Development of Lead-Free Interconnection Materials in Electronic

Materials & Design 215 (2022) 110439
Contents lists available at ScienceDirect
Materials & Design

journal homepage: www.elsevier.com/locate/matdes
Development of lead-free interconnection materials in electronic

industry during the past decades: Structure and properties
Su-juan Zhong a,c, Liang Zhang b,c,⇑, Mu-lan Li b, Wei-min Long c, Feng-jiang Wang d
a
School of Materials Science and Engineering, Henan University of Science and Technology, Luoyang 471000, China
b
School of Mechatronic Engineering, Jiangsu Normal University, Xuzhou 221116, China
c
Zhengzhou Research Institute of Mechanical Engineering Co., Ltd, Zhengzhou 450001, China
d
School of Materials Science and Engineering, Jiangsu University of Science and Technology, Zhenjiang 212100, China
h i g h l i g h t s g r a p h i c a l a b s t r a c t
The effect of different element or Sn-Cu-Ni-0.5CNTs-0.05GNSs/Cu interface.

particles on structure and properties
of Sn-based solder was summarized.
With the latest researches, the
mechanism of alloying element or
particles on the performances of lead-
free solder has been studied.
The reliability of of Sn-based solder
bearing various element or particles
has been sketched out.
a r t i c l e i n f o a b s t r a c t
Article history: During the past decades, series of lead-free solders have been developed rapidly, and are considered as
Received 19 August 2021 the attractive interconnection materials replacing traditional Sn-Pb solders in electronic industry. In this
Revised 26 December 2021 paper, the interfacial reaction, microstructure evolution, wettability, melting behavior, mechanical prop-
Accepted 29 January 2022
erties and reliability of lead-free solders/solder joints bearing alloying elements or particles were system-
Available online 3 February 2022
atically reviewed. The effect mechanism of alloying elements and particles on interfacial intermetallic
compound (IMC) layers and matrix microstructures were described. What’s more, the reaction precipita-
Keywords:
tion and solid solution precipitation have been demonstrated based on experiments. No obvious change
Lead-free solder
Alloying
of melting temperature can be found, suggesting that there is no need to change the soldering processing
Reaction precipitation when adopting these novel lead-free solders. About the wettability and mechanical properties of solders
Mechanical properties or solder joints bearing alloying element and particles, the enhance effect can be found. The reliability
Drop reliability assessments including fatigue behavior, drop reliability, humidity environment, electromigration prop-
erty and whiskers were all analyzed and reviewed, and the influence mechanism of alloying elements
and particles on the reliability needs to be further studied systematically, especially for the drop
⇑ Corresponding author at: School of Mechatronic Engineering, Jiangsu Normal University, Xuzhou 221116, China.
E-mail address: [email protected] (L. Zhang).
https://doi.org/10.1016/j.matdes.2022.110439
0264-1275/Ó 2022 The Authors. Published by Elsevier Ltd.
This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
Su-juan Zhong, L. Zhang, Mu-lan Li et al. Materials & Design 215 (2022) 110439
reliability and humidity environment. The reviews can provide the theoretical reference for the investi-
gation of lead-free solders in the future.
Ó 2022 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license
(http://creativecommons.org/licenses/by-nc-nd/4.0/).
Contents
1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
1.1. Interface reaction and growth . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
1.2. Sn-Ag-Cu solders . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
1.3. Sn-Ag solders . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
1.4. Sn-Cu solders . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9
1.5. Sn-Zn solders . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
1.6. Sn-Bi solders . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13
2. Microstructure evolutions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17
2.1. Sn-Ag-Cu solders . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17
2.2. Sn-Ag solders . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 22
2.3. Sn-Cu solders . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 24
2.4. Sn-Zn solders . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 25
2.5. Sn-Bi solders . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 29
3. Wettability . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 31
3.1. Contact angle of lead-free solders . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 31
3.2. Spreading ratio and spreading area of solders. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 31
3.3. Wetting balance testing of lead-free solders . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 31
3.4. Effects of alloying elements and particles on the wettability of lead-free solders . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 32
4. Melting behavior . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 34
5. Mechanical properties . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 34
5.1. Shear and tensile properties of lead-free solder joints . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 36
5.2. Hardness of lead-free solders . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 40
5.3. Creep behavior of lead-free solders . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 41
6. Reliability of lead-free solder joints . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 43
6.1. Fatigue reliability of lead-free solder joints in devices . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 43
6.2. Drop reliability of lead-free solder joints. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 47
6.3. Bending reliability of lead-free solder joints . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 48
6.4. Electromigration of lead-free solder joints . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 48
6.5. Reliability of solder joints under relative humidity environment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 49
6.6. Whiskers in lead-free solders . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 50
7. Conclusions. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 53
Declaration of Competing Interest . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 53
Acknowledgments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 53
Data availability . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 53
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 53
1. Introduction Agency, Waste Electrical and Electronic Equipment (WEEE) pieces

of legislation and European Union Restriction of Certain Hazardous
The use of solder materials has a long history due to the low Substances (RoHS) have banned respectively Pb-containing elec-
melting temperature (231.89 °C for pure Sn) and good soldering tronic products [5-7]. Then, the idea of being lead-free and envi-
properties. Dating back to the Bronze Age, the animal teeth ronmentally friendly has spread around the world. Therefore,
unearthed in Mesopotamia were connected by soldering. More- choose lead-free solder to replace the traditional Sn-Pb solders
over, soldering materials were found in Sanxingdui bronze ware has become an important research topic in the electronics indus-
and Jiuliandun bronze ware of Shang Dynasty in China [1,2], try, which also prompts worldwide research on Pb-free solders
demonstrating the solders have superior performance as the inter- for electronic interconnection.
connect material, and the application can be dated back to BC4000. To replace the traditional Pb-containing solders, researchers of
In recent decades, with the rapid development of electronic prod- all over the world put forward lead-free solders with different
ucts, the advantages of solders are further widely used in the elec- melting temperature, as shown in Fig. 1. Sn-Ag-Cu ternary alloys
tronic devices, especially for Sn-Pb. A series of Sn-Pb solders with are the most studied solders in the lead-free solder field. Sn-Ag-
different composition in electronic industries is selected for bond- Cu has been proposed by Japanese (Sn-3.0Ag-0.5Cu), EU (Sn-
ing electrical components and substrates to ensure the mechanical 3.8Ag-0.7Cu) and US (Sn-3.9Ag-0.6Cu) as replacement for the tra-
integration and electric connection of electronic devices [3,4].The ditional Sn-Pb solders [8]. Compared with Sn-Ag-Cu solder (217
reliability connection of electronic devices are realized by Sn-Pb °C), the melting temperature of Sn-Ag (221 °C) [9] and Sn-Cu
solder, and the performance of Sn-Pb solder joints is comprehen- (227 °C) [10] binary solder are relatively high, and they are widely
sively well understood. used in reflow soldering and wave soldering, respectively. For
However, because Pb is harmful to the environmental and Sn-Zn lead-free solders, the alloys become attractive as the low
human health, since 1 July 2006, U.S. Environmental Protection eutectic temperature (198 °C), which is obvious lower than that
2
Fig. 2. Typical interface reaction model.
reaction microstructure images, the interface phase is almost all of

Fig. 1. Several typical lead-free solders.
Cu6Sn5. Only when the heating time increases to a certain degree,
an obvious Cu3Sn layer in the interface can be observed. Fig. 3
shows the cross-section of Cu6Sn5/Cu3Sn layers of Sn-Cu, Sn-Cu-
of Sn-Ag-Cu ternary [11], The temperature is close to the eutectic Ni, Sn-Ag-Cu and Sn-Pb solder joints in BGA device. The SEM
temperature of Sn-Pb alloys (183 °C). It is demonstrated that the images show that the Cu3Sn layers can be formed between the
Sn-Zn lead-free can be selected to replace the Sn-Pb solders with Cu substrates and Cu6Sn5 layers, and Kirkendall voids can be
the reduction of cost. However, the poor wettability, weak oxida- observed in the Cu3Sn layers in the specimens aged [27].
tion resistance, low reliability will restrict the wide application of In order to analyze the IMC thickness variation of lead-free sol-
Sn-Zn in electronic industry [12]. For Sn-Bi solders, the melting der joints, the IMCs (Cu6Sn5 or Cu3Sn) growth is assumed to be
temperature (138 °C) is lower than that of traditional Sn-Pb sol- controlled by volume diffusion, and the growth rate is proportional
ders, and the cost is lower [13,14]. Therefore, Sn-Bi solder has to the square root of aging time [28,29]. The IMC thickness as a
become a research hotspot as interconnect material. In addition, function of the time can be expressed as Eq. (1).
Sn-In eutectic solder (118 °C) as a low temperature interconnect pffiffiffiffiffiffi
material is widely concerned. The great ductility, long fatigue life
Xt ¼ X0 þ Dt ð1Þ
and excellent wettability make it as a promising candidate for where X t is the IMC layer thickness at time t, X 0 is the initial IMC
lead-free solders [15]. For high temperature soldering in the man- layer thickness after soldering, and D is the diffusion coefficient as
ufacturing of power semiconductor packaging, Sn-Sb alloys with a function of temperature.
high creep-resistance and high strength have been selected to be The diffusion coefficient at different temperatures is often
utilized in the soldering processing [16,17]. The Sn-Sb alloys with found to be well predicted by
alloying have been investigated systematically [18-22]. In order
Q
to further promote the performances of lead-free solders, many D ¼ D0 exp ð2Þ
researchers adopted the methods of elements alloying [23,24] KT
and particle strengthening [25,26] to modify the lead-free solders, where Q is the activation energy of diffusion, K is the Boltzmann
significantly improving the wettability, mechanical properties, ser- constant (8.617 105 eV/K), and T is the temperature.
vice life, grain refinement, and inhibiting the growth of intermetal- From the measured thickness data, K can be determined for
lic compounds (IMCs). The increasing miniaturization of electronic each experimental temperature. Using Eq. (3), the activation
component, especially for three-dimensional integrated circuit (3D energy Q can be determined from the slope of the straight line
IC), has encourages the development of lead-free solders to meet obtained by plotting lnðDÞ against 1=T. Eq. (2) could then be
the requirements of metal interconnection. expressed as follows, by taking the logarithms of both sides of
For the series of lead-free solders, Sn-Ag-Cu, Sn-Ag, Sn-Cu, Sn- the equation.
Zn and Sn-Bi solders have been investigated and published with
so many literatures. In this paper, the development of the five Q
lnðDÞ ¼ lnðD0 Þ þ ð3Þ
kinds of lead-free solders in electronic industry during the past KT
decade, the effect of elements alloying and particle strengthening The activation energies Q can be calculated from the slope of the
on the interfacial reaction, microstructures, melting behavior, wet- Arrhenius plot using a linear regression model. Based on the calcu-
tability, mechanical properties and reliability of solders and solder lation using Eq. (1)-Eq. (3), the diffusion coefficient and activation
joints were summarized. energies can be calculate to analyze the effect mechanism of ele-
ments alloying or particles strengthening on the growth of IMC
1.1. Interface reaction and growth at the interfaces.
In the process of soldering, the molten solder contacts with the 1.2. Sn-Ag-Cu solders
metal electrode, the solder in the form of liquid, the electrode in
the form of solid, the liquid-solid diffusion reaction occurs. So Sn-Ag-Cu family are now commonly utilized for circuit board
the intermetallic compounds can be formed as reaction products assembly as replacements for the traditional eutectic Sn-37Pb sol-
between solder and metal electrode. Fig. 2 shows the schematic der [30]. The alloying elements of Sn-Ag-Cu lead-free solders have
illustration of typical interface reaction model. Taking Cu as exam- been investigated by many researchers. Rare earth elements are
ple, during reflow soldering, the solder melts and spreads on the considered as the ‘‘vitamin” of metals, meaning that a slight of rare
surface of Cu, and reacts with Cu to form scallop-type Cu6Sn5 earth elements can greatly improve the performances of metals
IMC. Due to the extremely short reflow soldering time, Cu3Sn is [31]. So the rare earth elements are considered as additives into
mostly less than 1 lm. Therefore, in the reflow soldering interface lead-free solders for electronic packaging [32]. The rare earth Ce
3
Fig. 3. Cross-section of Cu6Sn5/Cu3Sn layers in the samples aged at 125 °C for 1000 h: (a) Sn-Cu; (b) Sn-Cu-Ni; (c) Sn-Ag-Cu and (d) Sn-Pb [27].
element (0.02–0.5%) has been selected as additive into Sn-3.0Ag- is the driving force of IMC growth. The reaction of Sn and Pr to form
0.5Cu solder by Tu [33]. After reflow soldering at 260 °C, 0.5% Ce PrSn3 can decrease the activity of Sn at the Cu6Sn5/solder interface.
can reduce the thickness of IMC from 2.92 lm to 2.50 lm. The Moreover, the stable PrSn3 particles in the molten alloy play a role
samples were subjected to 180 °C thermal aging, and the morphol- as the heterogeneous nucleation sites and enhance the solidifica-
ogy gradually changes from scallop-type to layer-type. The addition of solder.
tion of Ce can slightly decrease the total thickness of IMC, For the investigation of Sn-3.0Ag-0.5Cu and Sn-3.0Ag-0.5Cu-
especially for Cu3Sn, which can be attributed to the formation of 0.3Ni solders [39], the IMC formation was analyzed on Cu, high
CeSn3 particles as diffusion obstacles to inhibit the formation and temperature treated Cu and graphene coated Cu substrates, respec-
growth of IMC. During thermal cycling and isothermal aging, as tively. The results indicates that the thickness of the (Cu, Ni)6Sn5
shown in Fig. 4, the kinetic analysis of IMC growth for Sn-3.8Ag- IMC layer of Sn-3.0Ag-0.5Cu-0.3Ni solder joint is higher than that
0.7Cu/Cu and Sn-3.8Ag-0.7Cu-0.03Ce/Cu solder joints was investi- of Sn-3.0Ag-0.5Cu solder joints. It is demonstrated that the addi-
gated by Zhang [34]. IMC growth rate for the two solder joints dur- tion of 0.3% Ni can increase the growth rate of IMC layer in Sn-
ing thermal cycling aging was higher than that during isothermal 3.0Ag-0.5Cu solder joints. The addition of Ga element can also
aging. The activation energy for the IMC (Cu6Sn5 and Cu3Sn) affect the IMC growth of Sn-Ag-Cu/Cu couple [40]. Due to the addi-
growth during aging is estimated to be 73.5 kJ/mol and 89.4 kJ/mol tion of 1.5 % Ga, the Cu atoms dissolve into the melting solder to
for Sn-Ag-Cu/Cu and Sn-Ag-Cu-Ce/Cu, respectively. In addition, the react with Ga element to form Cu2Ga layer, after 260 °C reflow sol-
IMC growth rate of Sn-Ag-Cu-Ce/Cu is smaller than that of Sn-Ag- dering, the thickness of Cu6Sn5 layer can be reduced significantly.
Cu/Cu. In particular, the addition of trace Ce into the Sn-Ag-Cu sol- Meanwhile, after aged at 180 °C for 4 days, Cu6Sn5/Cu3Sn layers
der can reduce the thickness of the IMCs of Sn-Ag-Cu/Cu solder can be observed and the thickness was decreased obviously,
joint. For Sn-0.7Cu, Zhao [35] found that with the addition of Ce, demonstrating that the Cu2Ga layer plays a diffusion barrier to
the increase of Ce content can reduce the average size, the aspect suppress the IMC growth of solder joints. The addition of
ratio and the thickness of the Cu6Sn5 grains on Cu substrates, while 0.5 % Ga can also be found the reduction of IMC growth in Sn-
can increase those of the IMC grains on the Ni substrate. For the 0.5Ag-0.7Cu-xGa/Cu solder joint [41]. In Sn-3.0Ag-0.5Cu/Cu solder
addition of Yb [36] or Pr [37], the suppression effects of IMC joints, 0.5%-1.5 % Ga can inhibit the IMC growth remarkably [42].
growth can also be observed. Gao [38] gives the potential explana- With the addition of 0.8% Zn into Sn3.8-Ag-0.7Cu solder joint
tion for the effect mechanism of rare earth element Pr on the IMC [43], significantly depressed growth of Cu6Sn5 layer can be
growth for Sn-Ag-Cu solder. Due to big difference of the atomic observed, which can be attributed to the effect of Zn addition in
radius between Sn and Pr, Pr tends to accumulate in the interface the alloy on the migration of Sn atoms toward the interface. Giu-
region. The Gibbs free energy 4G depended on the activity of Sn ranno [44] selected the Sb as the additive into Sn-2.0Ag-1.3Cu/
4
Fig. 4. Interfacial cross-section of solder joints: (a) Sn-Ag-Cu/Cu (300 thermal cycles); (b) Sn-Ag-Cu-Ce/Cu (300 thermal cycles); (c) Sn-Ag-Cu/Cu (300 h aging) and (d) Sn-Ag-
Cu-Ce/Cu (300 thermal cycles) [34].
(Cu,Ni) solder systems. Sb can reduce the thickness of the IMC layer ness is even during aging. The investigation shows that the addi-
formed at the interface. Moreover, the addition of Sb into Sn- tion of Cr can reduce the diffusion coefficient of Sn and Cu, and
3.5Ag-0.7Cu solder can reduce the Cu6Sn5 grains growth rate the Cr in the matrix can weak the reaction rate of Sn and Cu,

[45], the average radius c of the Cu6Sn5 grains can be calculated decreasing the growth rate of the interfacial IMC. P element was
using the Eq. (4) and Eq. (5). Additionally, the author has demon- selected by Chen [48] as additives into Sn-3.0Ag-0.5Cu. At the
strated that the diffusivity of Cu through channel in solder joints interface, the IMC layer, especially for Cu3Sn, the thickness at the
bearing 1.0% Sb is the lowest. Sn-Ag-Cu-P solder joints is greatly higher than that at the Sn-Ag-

Cu solder joints. The authors proposed that a small amount of P
c ¼ 0:913ðktÞ1=3 ð4Þ addition can accelerate the Cu-Sn diffusion flux through the Sn-
Ag-Cu/Cu interface, which can be attributed to the reaction
b e
9 n D C C d
between P and Cu, resulting in lowering the reaction opportunity
k¼ ð5Þ of Cu and Sn, and increasing the activity of Sn.
2 ni Ci
The nanoparticles added into lead-free solders can be selected
where t is reflow time; n is atomic density; ni is the atomic density as an effective way to modify the growth behavior of interfacial
in the Cu6Sn5 grain; D is the diffusivity of the Cu in the molten alloy; IMC layers. The Mo nanoparticles can reduce the IMC thickness
C b is the quasi-eqilibrium concentration of Cu in the vicinity of the and scallop diameter after reflow soldering at 250 °C. The author
Cu substrate; C e is the Cu concentration in the alloy melt in stable suggests that the nanoparticles tend to adsorb preferentially at
the Sn-Ag-Cu/Cu interface [49]. The effect of Ni nanoparticles on
equilibrium with a planar interface of Cu6Sn5; C i is the Cu concen-
the IMC growth between Sn-3.8Ag-0.7Cu solder and Cu substrate
tration in the scallop-type Cu6Sn5; d is the width of the channel
was studied by Tay [50]. An increase in the Cu6Sn5 thickness and
between Cu6Sn5 grains.
a decrease in the Cu3Sn was found with the addition of Ni nanopar-
The effects of Bi and In additions on IMC layers in Sn-3.7Ag-
ticles. Due to the addition of Ni nanoparticles, the Ni atoms entered
0.7Cu/Cu, Sn-1.0Ag-0.5Cu-1.0Bi/Cu and Sn-1.5Ag-0.7Cu-9.5In/Cu
^
the Cu sublattice of the Cu6Sn5 and substituted the Cu atoms to
A
lead-free solder joints are studied by Hodúlov a [46]. After 250 form (Cu, Ni)6Sn5 phase. So the Ni additive can increase the Cu6Sn5
°C reflow soldering, Cu6Sn5 and Cu6(Sn, In)5 layers can be observed, thickness, and make this phase more thermo-dynamically stable.
respectively. Cu3Sn can be observed during aging, and its growth So the reaction as shown in Eq. (6) can be suppressed, the Cu3Sn
can be decreased by Bi and In addition. Researchers suggested that thickness in the Sn-Ag-Cu solder joints can be reduced signifi-
Bi and In can substitute Sn in the IMC, Cu3(Sn, In) or Cu3(Sn, Bi) cantly. The Al nanoparticles have been selected as additive into
may form at the Cu3Sn grains boundaries, which can reduce the Sn-3.8Ag-0.7Cu solder joints [51]. Al nanoparticles can reduce the
diffusion of Sn at the interface. The effect of Cr element on the element diffusion coefficient at the Sn-Ag-Cu/Cu interface, so the
IMC layer of Sn-3.0Ag-0.3Cu/Cu interface [47] was investigated, thickness of Cu6Sn5 layer and Cu3Sn layer can be reduced during
as shown in Fig. 5. Comparing with Sn-Ag-Cu solder joints, the thermal cycles loading. Nano Mn particles can be also used to mod-
scallop-type Cu6Sn5 are smaller in the Sn-Ag-Cu-Cr solder joint. ified Sn-Ag-Cu solder in the industry [52]. With the addition of Mn
The morphology of IMC layer is regular wave-shape and the thick- nanoparticles, the morphology and IMC thickness can be changed.
5
Fig. 5. Cross section of IMC layer in solder joints: (a) Sn-Ag-Cu after soldering; (b) Sn-Ag-Cu after aging; (c) Sn-Ag-Cu-Cr after soldering and (d) Sn-Ag-Cu-Cr after aging [47].
When the 0.1% Mn was added, the IMC thickness can be reduced La2O3 [56] and Al2O3 [57] nanoparticles as additives into Sn-
slightly after reflow soldering and isothermal aging. Meanwhile, 3.8Ag-0.7Cu and Sn-0.3Ag-0.7Cu solders, respectively. The growth
the higher activation energy can be obtained. The author suggested rate of Cu6Sn5 and Cu3Sn can be suppressed significantlyThese
that the grain boundary pinning of Mn nanoparticles is the mech- nanoparticles are effective surface-active materials, adsorbing Sn
anism for IMC growth inhibition. Fe micro-particles were added atoms to hinder the diffusion of Cu and Sn atoms, which can induce
into Sn-3.0Ag-0.5Cu solder by Liu [53]. It is found that Fe particles the decrease of driving force for Cu-Sn IMC formation. For the
deposit in the vicinity of Cu6Sn5, the reaction between Fe and Sn application of oxide particles, NiO [58], SnO2 [59], Fe2O3 [60],
can be found, which can retard the growth of Cu6Sn5 and Cu3Sn CeO2 [61], ZnO [62], TiO2 [63], SiO2 [64], Y2O3 [65] nanoparticles
layers at Sn-Ag-Cu-Fe/Cu interface during liquid-state reaction were selected as additives for Sn-Ag-Cu solders, as shown in
and the growth of Cu3Sn during solid-state aging. Moreover, the Table 1. The IMC thicknesses were reduced to different degrees
roughness Rrms of the Sn-Ag-Cu-Fe/Cu interface can be determined during different temperature environments (reflow soldering,
using Eq. (7). Based on the determination of roughness, it is isothermal aging and thermal cyclic loading). Fig. 6 shows the
demonstrated that the roughness of IMC layer at Sn-Ag-Cu-Fe/Cu top-view of Cu6Sn5 grains variations with the addition of Y2O3
is much smaller than that of Sn-Ag-Cu/Cu. With the addition of nanoparticles, based on the measurement of Cu6Sn5 grains size,
Co nanoparticles [54], the IMC thickness of Sn-0.45Ag-0.68Cu/Cu the relationship between the average radiuses of Cu6Sn5 grains
was increased, due to the formation of (Cu, Co)6Sn5. and reflow soldering time can be fitted as Eq. (8) and Eq. (9). This
indicates that the Y2O3 nanoparticles can effective suppress the
Cu6 Sn5 þ 9Cu ! 5Cu3Sn ð6Þ
growth of Cu6Sn5 grains at the Sn-Ag-Cu/Cu interface. However,
vffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi Aspalter [66] gives different results. Ceramic nanoparticles
u N
u1 X 2 (Al2O3, SiO2, TiO2, ZrO2) were added to flux to reduce the growth
Rrms ¼t Z ð7Þ rate of Cu3Sn layer at Sn-3.0Ag-0.5Cu/Cu interface during 170 °C
n i¼1 i
aging, which indicates that the addition of oxide nanoparticles into
solder or into flux, the effect mechanism is different.
where N is the data number of Z i .
Fe2NiO4 nanoparticles were selected by Chellvarajoo [55] as
hri ¼ C 1 t 1=3 ð8Þ
additives into Sn-3.0Ag-0.5Cu solder joints. The morphology of
Cu6Sn5 layer can be changed from scalloped-structure to continu-
ous planar type after 260 °C reflow soldering. The thickness of hri ¼ C 2 t 1=6 ð9Þ
the Cu6Sn5 and grain structures can be reduced with the increase
content of Fe2NiO4 nanoparticles. During thermal loading, for where C 1 and C 2 are the constant.
6
Table 1
Effect of elements and particles on the growth of Cu-Sn IMC
Composition Additives Content Reflow Prolonged soldering Thermal aging Thermal cycling Processing Reference
(wt.%) soldering Temperature
Cu6Sn5 Cu3Sn Cu6Sn5 Cu3Sn Cu6Sn5 Cu3Sn Cu6Sn5 Cu3Sn
Sn3.0Ag0.5Cu Ce element 0.02–0.5 180 °C aging [33]
260 °C reflow
Sn3.8Ag0.7Cu Yb element 0.05 245 °C reflow [36]
Sn0.3Ag0.7Cu Pr element 0.05 150 °C aging [37]
Sn3.0Ag0.5Cu Ni element 0.3 260 °C reflow [39]
Sn3.5Ag0.7Cu Ga element 1.5 260 °C reflow [40]
180 °C aging
Sn3.8Ag0.7Cu Zn element 0.8 245 °C reflow [43]
Sn3.5Ag0.7Cu Sb element 0.5–2.0 250 °C reflow [45]
Sn1.0Ag0.5Cu Bi element 1.0 250 °C reflow [46]
150 °C aging
Sn1.5Ag0.7Cu In element 9.5 250 °C reflow [46]
150 °C aging
Sn3.0Ag0.3Cu Cr element 0.05 260 °C reflow [47]
150 °C aging
Sn3.0Ag0.5Cu P element 0.5 [48]
Sn3.8Ag0.7Cu Nano-Mo 0.1 250 °C reflow [49]
Sn3.8Ag0.7Cu Nano-Ni 0.27 75 °C,100 °C,125 [50]
°C,150 °C,175 °C
aging
Sn3.8Ag0.7Cu Nano-Al 0.1 fx2 250 °C reflow [51]
55 °C – 125 °C
Sn0.3Ag0.7Cu Nano-Mn 0.1 Near 250 °C [52]
reflow, 100 °C, 150
°C , 190 °C aging
Sn3.0Ag0.5Cu Micro-Fe 0.5,1.0 v 250 °C reflow [53]
150 °C aging
Sn0.45Ag0.68Cu Nano-Co 1.0 240 °C, 250 °C [54]
reflow
Sn3.0Ag0.5Cu Nano-Fe2NiO4 0.5–2.5 260 °C reflow [55]
Sn3.8Ag0.7Cu Nano-La2O3 0.1 55 °C – 125 °C [56]
thermal cycles
Sn0.3Ag0.7Cu Nano-Al2O3 0.12 55 °C – 125 °C [57]
thermal cycles
Sn3.0Ag0.5Cu Nano-NiO 0.5–2.5 Reflow soldering [58]
Sn1.0Ag0.7Cu Nano-SnO2 0.3–1.3 300 °C reflow [59]
(Total) 150 °C aging
Sn3.0Ag0.5Cu Nano-Fe2O3 0.01–0.15 239 °C reflow [60]
Sn3.0Ag0.5Cu Nano-CeO2 1.0 (Total) 230 °C,250 °C,270 [61]
°C reflow
Sn3.0Ag0.5Cu Nano-ZnO 0.5–2.0 255 °C reflow [62]
(Total) 170 °C aging
Sn3.0Ag0.5Cu Nano-TiO2 0.05–0.6 242.9 °C reflow [63]
Sn3.0Ag0.5Cu Nano-SiO2 0.05–1 250 °C reflow [64]
(Total) 55 °C – 125 °C
thermal cycles
Sn3.0Ag0.5Cu Nano-Y2O3 0.1 240 °C reflow [65]
Sn3.0Ag0.5Cu Nano-ceramic 0.5,1.0 170 °C aging [66]
Sn3.8Ag0.7Cu Micro-CuZnAl 0.5 250 °C reflow [67]
Sn3.0Ag0.5Cu Fullerene 0.05–0.2 150 °C aging [69]
Sn3.0Ag0.5Cu Nano-TiC 0.05–0.2 150 °C aging [69]
Sn3.0Ag0.5Cu Ni-GNS 0.05–0.2 150 °C aging [69]
Sn3.0Ag0.5Cu Ni-CNTs 0–0.2 250 °C reflow [70]
150 °C aging
For the addition of 0.5% CuZnAl micro-particles into Sn-3.8Ag- 0.5Cu/Cu can be reduced significantly. Ni modified carbon nan-
0.7Cu solder joints [67]. It is found that the 0.5% CuZnAl micro- otubes (Ni-CNTs) was manually mixed into Sn-3.0Ag-0.5Cu solder
particles can reduce the Cu6Sn5 and Cu3Sn layers in the solder [70], which can prevent the formations of Cu6Sn5 and Cu3Sn at Sn-
joints, and decrease the formation of voids, which can be attributed 3.0Ag-0.5Cu/Cu interface. In addition to adding alloying elements
to nucleation particles mechanism of CuZnAl. The particles can and nanoparticles, the rapid growth of interfacial IMC layers can
increase nucleation rate and refine the IMC grains sizes. Moreover, be inhibited by changing the metal pad. Electroless nickel/immer-
the interfacial IMC layer was also investigated for Sn-3.8Ag-0.7Cu sion silver (ENImAg) can be developed as an alternative surface fin-
and Sn-3.8Ag-0.7Cu-0.5CuZnAl on Fe substrate [68]. The 0.5% CuZ- ish on Cu pad for Sn-Ag-Cu solders [71]. The results indicate that
nAl micro-particles can decrease the growth rate the FeSn2 IMC the thinner layer and smaller grain sizes can be observed on the
layer, which further improve the inhibition mechanism of CuZnAl ENImAg surface finish than that on bare Cu. With the addition of
on the IMC layer. For the addition of fullerene, TiC and Ni-GNS Zn into Cu substrate can suppress the formation of large Ag3Sn
nanoparticles [69], the thickness of Cu3Sn layer of Sn-3.0Ag- plate and growth of IMC layers [72].
7
Fig. 6. Top-view of interfacial Cu6Sn5: (a) Sn-Ag-Cu, 2 min; (b) Sn-Ag-Cu, 5 min; (c) Sn-Ag-Cu, 15 min; (d) Sn-Ag-Cu-Y2O3, 2 min; (e) Sn-Ag-Cu-Y2O3, 5 min and (f) Sn-Ag-Cu-
Y2O3, 15 min [65].
1.3. Sn-Ag solders interfacial area. Moreover, long and hexagonal Cu6Sn5 can be found
near the interfacial IMC layer.
Sn-Ag solders can also be considered as an important intercon- Tu [78] has introduced that Sn-Ag micro-bumps were used to
nection materials for electronic devices. Sn-2.3Ag [73] and Sn- interconnect the stacking chips on Cu UBM 10 lm thick layer of
3.5Ag [74] alloys have been utilized in electronic devices (FCBGA, Sn-Ag micro-bumps and the schematic diagram of the micro-
CSP). The interface reaction of Sn-Ag solder on different finishes bump, as shown in Fig. 8. After reflow and storage, Sn whiskers
materials has been investigated systematically. can be observed on the cap surface. When the Sn whisker grows
The 3D IC is becoming an attractive technology in electronic long enough, it will connect the adjacent micro-bumps and cause
industry. It is regarded as a solution in semiconductor for the a short circuit in the whole structure. Based on thick optimization
new generation electronic products due to its higher packaging design, the whisker growth can be reduced obviously. With the
densities, better performance and smaller feature sizes. In 3D chip EBSD testing, the Cu6Sn5 grains and the orientation can be deter-
stacking packaging, the IMC solder joints have been proposed to mined. Before reflow, the IMC can be found, after a long time of
meet the reliability requirement of structure [75]. Chen [76] interface reaction, the upper and lower layers of intermetallic com-
assessed the growth reaction of Ni3Sn4 IMC during bonding with pounds contact each other, forming a complete intermetallic com-
Sn-2.5Ag solder. Fig. 7 shows the 3D advanced chip stacking pack- pound solder joint.
aging with Sn-Ag/Ni/Cu solder joints. The Ni3Sn4 formation In order to enhance the microstructure of Sn-Ag solders, Zn was
between the Sn-2.5Ag and Ni/Cu layers can realize the chip stack- selected to modify the interface microstructure by Luo [79]. Inter-
ing after 250 °C bonding. With the increasing of bonding time, the face reaction of Sn-xAg-1Zn/Cu and Sn-2Ag-xZn/Cu (x = 1, 2, 3) sol-
thicker IMC can be found with the morphology variation from der joints was investigated systematically. The Cu6Sn5 and Cu5Zn8
sharp shape to rounded shape. Sn-3.5Ag also be used in 3D packag- particles can be observed at the Sn-xAg-1Zn/Cu interface after
ing with different electroplating layer structure (Ag/Sn, Sn/Ag, Ag/ reflow soldering. Moreover, for Sn-2Ag-xZn/Cu solder joints, when
Sn/Ag) on Cu substrate [77]. For the Sn/Ag structure, Cu6Sn5 with the Zn content is more than 2.0%, Ag5Zn8 particles grow on inter-
smooth and continuous morphology can be observed. For Ag/Sn, face, and the IMC layer is thinner than Sn-xAg-1Zn/Cu solder joints.
Ag/Sn/Ag structure, the thinner Cu6Sn5 layers were formed in the The addition of rare earth La can also improve the metallurgical
8
Fig. 7. 3D advanced chip stacking packaging with Sn-Ag/Ni/Cu solder joints [76].
Fig. 8. Schematic diagram of the Sn-Ag micro-bump and the interface reaction [78].
reaction of Sn-Ag/Cu solder joints [80]. The LaSn3 can be found near formation and growth behavior of Cu6Sn5 IMC [81]. The results
the IMC interface layer of Sn-3.5Ag-1.0La/Cu solder joints. After demonstrated that the addition of Cu can increase the thickness
150 °C aging with 625 h, it is found that the addition of La can sup- of Cu6Sn5 IMC layer, which can be attributed to the fact that the
press the IMC growth. For Sn-3.5Ag/Cu solder joints, the thickness Cu6Sn5-type medium-range order clusters provided potential
of Cu6Sn5 layer is 5.9 lm. For Cu3Sn, it is 2.8 lm. For Sn-3.5Ag- nuclei for the formation of Cu6Sn5 and thus facilitated its growth.
1.0La/Cu solder joints, the Cu6Sn5 thickness is 3.8 lm. Cu3Sn has
a thickness of around 2.5 lm. The phase and orientation of the 1.4. Sn-Cu solders
Sn-3.5Ag-1.0La solder was shown in Fig. 9. The images plot that
LaSn3 particles are randomly distributed within the Sn grains or Sn-Cu lead-free solder is a Sn-based lead-free solder that has
eutectic zone. Some particles are observed to be accumulated at been used extensively in the electronic packaging industry [82].
the grains boundaries. The LaSn3 particles can act as the heteroge- Sn-Cu has the advantages of low cost and the excellent perfor-
neous nucleation sites in the solder matrix, which can induce the mance [10]. For 270 °C and 298 °C reflow soldering carried out
refining effect of the microstructures. Sn-3.5Ag-xCu(x = 0, 0.7 by Satyanarayan [83], needle-like and thick protruded Cu6Sn5 can
and 1.5) solders on Cu substrate after reflow soldering were stud- be observed at Sn-0.7Cu/Cu interface. Only at 298 °C the Cu3Sn for-
ied to analyze that the effect of Cu on the liquid structure on the mation on Cu substrate can be found. At Sn-0.7Cu/Cu interface
9
Fig. 9. EBSD of Sn-3.5Ag-1.0La solder: (a) Ag maps and grains boundaries; (b) Sn inverse pole figure maps for the sample normal direction and (c) LaSn3 inverse pole figure
maps for the sample normal direction [80].
respond to the polymorphic transformation of Cu6Sn5, and may be

indicative of transformation-related stresses.
When new elements are added into the Sn-Cu solder, the new
elements participate in the metallurgical reaction, which can
change the types of intermetallic compounds in the solder joints.
For example, when Au was added into Sn-Cu solders, the Au-Sn
IMC can be found in the solder joints. Fig. 11 shows the phase dia-
gram of Sn-Cu-Au ternary system at 200 °C [85]. Zn and Ga were
simultaneously added into Sn-0.7Cu solder joints [86]. Based on
the study of interfacial structure of the solder/ENIG, the investiga-
tion demonstrated that the Ga can slightly change the morphology
and growth orientation of IMC layer. However, the Zn can dissolve
into interfacial layer to form (Cu, Ni)6(Sn, Zn)5. In Hasnine’s work
[87], the positive effect of Ga has also been proved. The Cu6Sn5
layer of Sn-Cu/Cu solder joints were refined and reduced in thick-
ness with the addition of Ga. The author suggested that Ga can
reduce the activity of Sn, and Cu can slow the Cu6Sn5 growth and
reaction at the Sn-Cu/Cu interface. Kadoguchi [88] proposed to
Fig. 10. TEM microstructure at Sn-0.7Cu/Cu interface (210 °C) [84]. add Cu balls (40–80 lm diameters) into Sn-0.7Cu solders. It is
found that 2.5% Cu balls can prompt the formation of a continuous
(Cu, Ni)6Sn5 IMC layer at the electrolytic Ni and the electroless Ni-P
[84], polymorphic phase transformation from monoclinic Cu6Sn5 to plating. Based on the high temperature storage testing at 200 °C for
hexagonal Cu6Sn5, and stress accumulation/release in Cu6Sn5 can 1000 h, the (Cu, Ni)6Sn5 IMC layer can work well as a Ni diffusion
be observed using in situ TEM. Fig. 10 shows the still-frame barrier.
in situ TEM images of Cu/Cu3Sn/Cu6Sn5/Sn-0.7Cu interface at 210 Zhao [89] has studied the effect of rare earth Ce on the interfa-
°C. In a temperature range the patterns appear that is likely to cor- cial reaction of Sn-0.7Cu/Cu and Sn-0.7Cu/Ni. With the increase of
10
0.7Cu-xIn/Cu after reflow soldering. With the addition of 1.0 wt%

In, some needle-like IMCs can be observed at the Sn-0.7Cu-1.0In/
Cu interface with much larger than the granular ones. Moreover,
when the In content is 5.0%, more needle-like IMCs can be found
at the interface. It is interesting to found that the increase of In
can increase the solubility of In in Cu6(Sn, In)5 IMC layers. In atomic
flux at the solder/Cu6Sn5 interface can be used to the effect of In
using Fick’s laws, as Eq. (10). With the increase of In content, the
@C=@x increases obviously, and more In atoms can be detected in
the Cu6(Sn, In)5 phase. The author considers Cu6(Sn0.89, In0.11)5
with the maximal solubility of In. Hanim [94] investigated that
the effect of rice husk ash (RHA) on the IMC at the Sn-0.7Cu-
xRHA/Cu (or ENIAg) interface. Thickness of the Sn-0.7Cu/Cu inter-
face layer was reduced from 7.45 lm to 6.13 lm by 0.01 RHA. Fur-
ther increasing of the RHA content can increase the IMC thickness,
which demonstrates that 0.01% RHA can effective inhibit the Cu/Sn
atoms diffusion, degrading the growth of Cu6Sn5 and Cu3Sn. More-
over, obvious reduction in IMC thickness within a range of 3.81–
4.74 lm was showed by the Sn-0.7Cu-xRHA/ENIAg as compared
Fig. 11. Isothermal section of the Sn-Cu-Au ternary system at 200 °C [85]. to the higher range of 6.13–9.3 lm showed by the Sn-0.7Cu-
xRHA/Cu.
Ce content, the average size and the aspect ratio of the Cu6Sn5 J ¼ Dð@C=@xÞ ð10Þ
grains were reduced, and the IMC layer thickness was decreased Where J is the In atomic flux at solder/Cu6Sn5 interface; D is the dif-
obviously for Sn-0.7Cu/Cu solder joints. However, the IMC layer fusion coefficient of In atom; @C=@x is the In atomic concentration
thickness was increased with the increase of Ce content for Sn- gradient.
0.7Cu/Ni solder joints. Bi as additives into Sn-0.7Cu solders [90]
can inhibit the growth of Cu3Sn at Sn-0.7Cu/Cu solder joints. The 1.5. Sn-Zn solders
growth behavior of IMC between the Sn-0.7Cu-xNi (x = 0, 0.1,
0.25, 0.5 and 1.0%) solders and Cu substrate was investigated to For Sn-Zn solder with 198.6 °C eutectic melting point, this lead-
analyze the effect of Ni addition on the interfacial IMC [91], with free solder has become a widely studied interconnect material in
the addition of the Ni, in the Sn-Cu/Cu interface, the IMC thickness electronic packaging [12,95]. The effect mechanism of Zn on the
increases obviously, the (Cu, Ni)6Sn5 layer can be observed at the interfacial microstructure Sn-xZn/Cu (x = 0, 0.2, 0.5 or 0.8%) solder
IMC layer. In addition, the sizes of the IMC grains for Sn-Cu/Cu joints by Chen [96]. For Sn/Cu solder joints, a large number of voids
bearing Ni are smaller than that for Sn-Cu/Cu solder joints. The can be found at the Cu3Sn/Cu interface. With the addition of Zn, the
addition of Ni can provide new more nucleation of the growth thickness of Cu3Sn can be reduced obviously. Adding 0.5% and 0.8%
for the IMC grains. Co as additives can also increase the thickness Zn can make the void in the interface completely disappear, which
ofCu6Sn5IMC layer in Sn-Cu/Cu solder joints [92]. Fig. 12 shows can be attributed to the suppression effect of Zn on the unbalanced
the interface microstructures of Sn-0.7Cu-0.04Co/Ni after 180 °C diffusion of Cu and Sn fluxes at the interface. With the addition of
aging for 520 h and Sn-0.7Cu-0.04Co/Cu after 150 °C aging for Zn, Zn atoms can served as diffusing species and participate at the
690 h. With the addition of Co, Co will participate in the interface Sn-xZn/Cu interface. Eq. (11) can be used to describe the interdif-
reaction to form intermetallic compounds containing Co. The addi- fusion. Fig. 14 shows the effect mechanism for retardation of void
tion of Co can inhibit the growth of Cu3Sn IMC layer, and reduce growth for Sn-xZn/Cu solder joints using density functional theory,
the number of Kirkendall voids. the fluxes of Cu and Sn via the IMCs layers were balanced out, and
The effect of In as additives on the interfacial IMC between Sn- the formation of voids at the interface was suppressed.
0.7Cu-xIn (x = 0–5.0 wt%) and Cu substrate was investigated by
Tian [93]. Fig. 13 shows the interfacial microstructures of Sn- J v ¼ J Cu þ J Sn þ JZn ð11Þ
Fig. 12. Interfaces of Sn-0.7Cu-0.04Co solder joints: (a) 180 °C for 520 h and (b) 150 °C for 690 h [92].
11
Fig. 13. Interfacial microstructures of Sn-0.7Cu-xIn/Cu after reflow soldering: (a)-(c) Sn-0.7Cu; (d)-(f) Sn-0.7Cu-1.0In and (g)-(i) Sn-0.7Cu-5.0In [93].
Fig. 14. Effect mechanism for retardation of void growth for Sn-xZn/Cu solder joints [96].
12
where Jv is the diffusion flux of vacancies; JCu , J Sn and JZn are the dif- (x = 0, 1, 4) solder joints. When the content of Cu is 7–10%, Cu6Sn5/
fusion fluxes of Cu, Sn and Zn, respectively. AuSn and (Cu, Au)Sn/AuSn can be formed at the Sn-Zn-7Cu/Au and
Rare earth Nd has been selected as additive into Sn-9Zn solder Sn-Zn-10Cu/Au interfaces. For Sn-8Zn-3Bi solder, 0.5% and 1% Cu
joints for enhancement by Hu [97]. To study the interface can decrease the IMC thickness, and enhance the activation energy
microstructures of Sn-9Zn/Cu and Sn-9Zn-0.06Nd/Cu solder joints of IMC growth, which indicates that the Cu can effectively inhibit
with 150 °C aging for different times, Cu5Zn8 IMC can be observed the growth rate of IMC layer [108].
at the interface. The IMC thickness increased with the increase of For Sn-Zn solder on aluminum alloy substrates [109], some
aging time, and the 0.06% Nd can repress the thickness of Cu5Zn8 micro-voids can be formed at the interface. With the addition of
IMC layer. Due to the high-active of Nd, NdSn3 can be formed Al2O3 nanoparticles, no defects such as micro-voids can be
and agglomerate at the grain boundary and interface, which can observed, meaning that the existence of Al2O3 nanoparticles can
induce the reduction of Cu5Zn8 growth rate at Sn-Zn/Cu interface. change the diffusion process during soldering, inducing the lack
Al and Ag elements can also modify the interfacial reaction of of Kirkendall micro-voids. Moreover, the results can demonstrate
Sn-Zn-x(Al, Ag) near-eutectic solders on Al and Cu substrates that the thickness of Al8ZnSn4 solid solution layer can be reduced
[98]. Al4.2Cu3.2Zn0.7 IMC layer can be observed at Sn-Zn-x(Al, Ag)/ from around 2.36–1.36 lm. The morphology of Al8ZnSn4 can be
Cu interface, and Al-rich (Zn) solid solutions at Sn-Zn-x(Al, Ag)/Al changed from scallop-shape to flat shape. The Al2O3 can act as
interface. However, different results can be found in Sn-Zn-xAg/ the nucleating agent role and promote heterogenous nucleation.
Cu solder joint. Ag5Zn8 can precipitate obviously as discrete nod- The theory of adsorption [110] can be used to analyze the effect
ules on Cu5Zn8 for Sn-Zn-xAg/Cu solder joints. Eq. (12) shows the mechanism of Al2O3 nanoparticles, as Eq. (13)-Eq. (16). In order
subsequent peritectic reaction [99]. Wang [100] tried to add to decrease the surface free energy, more Al2O3 nanoparticles
0.24% Al into Sn-Zn solder, and found that the IMC thickness can should be adsorbed on the crystal surface, to maximize the value
be decreased obviously. However, due to the small amount addi- of CK .
tion of Al, Al4.2Cu3.2Zn0.7 IMC was not found.
K
C dc
CK ¼ ð13Þ
RT dC
L + c-Ag5 Zn8 ! e-AgZn3 ð12Þ
where CK is the amount of adsorption of surfactant on crystal sur-
Sn-Zn bearing 0.5 % Ga or 0.2% Na on Al and Ni substrates were
face K; C is the total concentration of surfactant; T is the absolute
investigated by Gancarz [101]. On Ni substrate, the Ni5Zn21 IMC
layer can be observed. Similar thickness of Sn-Zn-0.2Na and Sn temperature; R is the ideal gas constant; cK is the surface tension
Sn-Zn-0.5 Ga was obtained, and grain boundary process was con- of crystal surface K.
sidered to control the growth rate of IMC. Moreover, no interlayer From the integral of the Eq. (13), the surface tension of crystal
can be formed on the Al substrate. However, the interface reaction surface K with the adsorption of Al2O3 nanoparticles can be
of Sn-Zn solder on Al and Ni substrates is not mentioned, so the expressed as Eq. (14).
influence mechanism of Ga and Nd on the interface cannot be dis- Z C
CK
cussed. The interfacial microstructures of Sn-Zn-xGa solders on Cu cKC ¼ cK0 RT dC ð14Þ
C
substrate were investigated by Chen [102]. With the addition of 0
1.0 % Ga, the thickness of Cu5Zn8 IMC layer is about the three times
of that of Sn-Zn/Cu solder joints, which demonstrates that the where cKC is the surface tension with adsorption of nanoparticles; cK0
addition of Ga can promote the growth rate of Cu5Zn8 layer of is the surface tension without adsorption. Eq. (15) represents the
Sn-Zn/Cu solder joints. Different effects can be proposed for In as surface energy of the final crystal.
0 1
additive into Sn-Zn solder [103]. On Cu and Ni substrates, Cu5Zn8
X X Z
@c RT
C
CK
and Ni5Zn21 IMCs layer can be found. Moreover, with the addition c K
C AK ¼ K
0 dC AAK ð15Þ
of In, the IMC thickness can be reduced obviously. K K
C
0
Compared with the interfacial microstructure of Sn-Zn/Cu and
Sn-Zn-0.1Cr/Cu solder joints [104]. After soldering at 240 °C for where AK is the surface are of crystal surface K. By Eq. (16), the min-
3 min, the IMC thickness at Sn-Zn/Cu interface was about 4– imum surface free energy can be obtained.
6 lm. With the addition of 0.1% Cr, the thickness of IMC layer Z
X C
CK
was reduced to about 2–3 lm. This also indicates that the addition AK dC ! max ð16Þ
of 0.1% Cr can significantly inhibit the growth of IMC layer. The K
C
0
effect of In as additives on the IMC layer of Sn-8Zn-3Bi/Cu was
investigated by Liu [105]. It can be found that the addition of In
can induce the slight increase of the IMC thickness. In as additive 1.6. Sn-Bi solders
can reduce the melting temperature of Sn-8Zn-3Bi solder on Cu
substrate, during reflow soldering. A longer molten period will be Sn-Bi lead-free solders, especially for the eutectic Sn-58Bi alloy
experienced for solders bearing In, which can give enough time with low melting temperature (138 °C), have a good application
for the interfacial reaction. Ag and Ni nanoparticles can also modify prospect in the soldering for the thermo-sensitive parts [111]. In
the interfacial IMC microstructure of Sn-8Zn-3Bi solder on OSP-Cu package-on-package (POP) processing, Sn-58Bi and Sn-3.0Ag-
substrate [106]. The addition of Ag nanoparticles can induce the 0.5Cu were united as composite solders to improve the technology
formation of AgZn3 IMC layer at the top surface of the scallop- [112]. Effect of 0.5 wt% La addition on the interfacial microstruc-
shaped Cu5Zn8 IMC layer at Sn-8Zn-3Bi/Cu interface. Ni nanoparti- ture of Sn-58Bi solder joint with Au/Ni/Cu pads [113] has been
cles can result in the formation of a ternary (Cu, Ni)-Zn IMC layer. studied. It is found that the IMC thickness of Sn-Bi-0.5La solder
The addition of Ag and Ni nanoparticles can reduced the IMC joints is much thinner than that of Sn-Bi solder joints, which shows
growth at the interface compared to the Sn-8Zn-3Bi/Cu solder that the La can depress the IMC growth due to the high chemical
joints. The interfacial microstructure of Sn-Zn-xCu (x = 0,1,4,7 or activity of rare earth La, causing it to segregate at the interface
10%) solder on Au substrate was studied by Yen [107]. The Cu con- and decrease of the interfacial energy. The influence of Ag addition
tent can influence the composition of IMC layer at the interface. into Sn-58Bi/Cu solder joints was studied by Hu [114]. During the
Au-Sn and Au-Zn-Sn IMC can be observed in Sn-Zn-xCu/Au soldering and aging process, Ag element in eutectic Sn-Bi solder
13
can diffuse into Cu substrate, forming a Cu-Ag layer at Sn-Bi-Ag/Cu Due to the curvature difference of IMC particles, the discrep-
interface. The addition of Ag has no obvious influence on the thick- ancy can result in the concentration gradient of solute atoms in
ness of the IMC layer at the interface, but can significantly induce the melt solder among different radius grains. As a result, the
the variation of IMC morphologies. higher concentration on the surface of small grains and lower con-
Effects of Zn on the interfacial microstructure and IMC growth centration on the surface of large grains can be found. The concen-
of Sn-58Bi-xZn/Cu (x = 0.1, 0.7 and 2.0 wt%) solder joints were tration discrepancy can induce movement of solute atoms from
investigated by Ma [115] aging at 180 °C for 400 and 900 h. A Cu6(- small grains to large grains, which can prevail the growth of large
Sn,Zn)5 layer can be observed at the Sn-58Bi-0.1Zn/Cu interface grains and the shrinkage or disappearance of small grains. The
after aging for 400 h. Then a Cu3(Sn,Zn) layer can be formed spacing between the grains can determine the growth rate of
between Cu6(Sn,Zn)5 layer and Cu substrate. With the addition of grains. Moreover, the ith Cu6Sn5 grain and its nearest grains can
0.7% Zn, CuZn phase can be found at the interface. Sn-rich layer be utilized for investigation to obtain the ripening flux of solute
cam ne observed between the CuZn and Cu6(Sn,Zn)5. 2.0% Zn will atoms between adjacent grains. Because the grains are relatively
induce the formation of Cu5Zn8 layer, and 0.5 wt% CuZnAl shape close, the size (average distance d) is significantly smaller than
memory alloy particles (2–6 lm) were selected as additives into the grain radius r. Therefore, the diffusion flux field of adjacent
Sn-58Bi solder. The findings demonstrated that the IMC growth grains are superimposed on each other, and the trend of diffusion
rates at Sn-Bi/Cu and Sn-Bi-0.5CuZnAl/Cu interfaces at 250 °C are or growth depends mainly on the surrounding grains. Using steady
higher than that of 230 °C. It is found that the CuZnAl particles state approximation, the flux of solute atoms since the different
can decrease the diffusion coefficient of IMC [116]. Ripening theory radius of IMC particles can be describes as follows:
can be utilized in the effect mechanism of CuZnAl particles on the
IMC of Sn-Bi-0.5CuZnAl/Cu solder joints. Fig. 15 shows the IMCs dC C C i
J R ¼ D ¼ D ð19Þ
morphology of Sn-Bi/Cu and Sn-Bi-0.5CuZnAl/Cu solder joints. dx d
The results indicate that the scallop-like Cu6Sn5 IMCs precipitate where d is the average distance between grains; D is the diffusion
firstly from the matrix microstructure, and the morphology of Cu6- coefficient of solute atoms in the molten solder.
Sn5 becomes rougher in service. The Ostwald ripening theory can
2McC 0 1 1
be utilized to explain the phenomenon [117]. The ripening model C C i ¼ ð20Þ
was shown in Fig. 15. Eq. (17) shows the Gibbs-Thomson equation RT q r r i
selected to analyze the Cu6Sn5 growth process.
2M cC 0 1 1 1
2Mc JR ¼ ð21Þ
C r ¼ C 0 exp ð17Þ RT q d r r i
RT qc

2M c where r i is the radius of the ith grain;r is the average radius between
If RT qc
1, C r can be approximately describe as follows:
grains d is the average distance between grains.
2M c From Eq. (21), six parameters of coarsening flux can affect the
Cr ffi C0 1 þ ð18Þ
RT qc transverse coarsening growth rate of scallop-like grains. The six
parameters are soldering temperature T, diffusion coefficient D,
where C 0 is the equilibrium concentration of Cu atoms in Sn-Bi or
Sn-Bi-0.5CuZnAl solders; M is the Cu6Sn5 molar volume; c is the average grain distance d, saturated solubility of solute Cu in liquid
interfacial energy per unit area between IMC and molten solder; T solder C 0 , average grain radius of ith grain radius r i , respectively.
is the absolute temperature; R is the gas constant; q is; density. For Sn-Bi/Cu and Sn-Bi-0.5CuZnAl/Cu solder joints, because the
Fig. 15. Ripening model of Sn-Bi/Cu and Sn-Bi-0.5CuZnAl/Cu: (a) illustration of concentration difference between grains; (b) Sn-58Bi-CuZnAl/Cu; (c) Sn-58Bi /Cu [116].
14
CuZnAl memory particles have little effect on the melting temper- [121]. Compared with Sn-Bi/Cu solder joints, the IMC growth of
ature of Sn-Bi solder, the similar temperature can be chosen for Sn-Bi-Mo/Cu solder joint is slower during thermal cycling. The
reflow soldering with the two solders. With the same reflow sol- results indicate that the excess growth of IMCs at the Sn-Bi/Cu
dering temperature, the same value can be found for the saturated interface is suppressed with the addition of Mo nanoparticles. So
solubility of Cu atoms in liquid Sn, all of which is 4.7 at.%. For the the reliability of Sn-Bi/Cu solder joints bearing Mo nanoparticles

can be improved. Ag nanoparticles were added into Sn-Bi solder
six parameters of coarsening flux, three grain parameters (d,r and
to analyze the interfacial reaction [122]. Due to the addition of
r i ) and diffusion coefficient D can affect the ripening flux (J R ) of IMC
Ag, Ag can react with Sn to form Ag3Sn, as barriers to block the dif-
at Sn-Bi/Cu and Sn-Bi-CuZnAl/Cu interfaces (250 °C, 10 min). The
fusion of metal atoms during current stressing. But for the Ag ele-
diffusion coefficient calculated using Eq. (1) are 0.01462 and
ment as additives into Sn-Bi solder, the IMC thickness of the
0.00767, respectively. The grains parameters d,r and ri can be mea- interface reaction can not show obvious variation [123]. For high
sured from Fig. 15, ripening flux (J R ) relationship between Sn-Bi/Cu temperature electronics, Jung [124] developed a fluxless and
and Sn-Bi-CuZnAl/Cu as Eq. (22) can be found. The results indicate binder-free paste comprising Cu nanoparticles. Sn-58Bi and
that the coarsening flux of Sn-Bi solder joint is 3.2 times that of Sn- polyvinylpyrrolidone dispersing agent, the schematic diagrams
Bi-0.5CuZnAl solder joint, showing that the coarsening degree of were shown in Fig. 16. During bonding procedure, the reaction
Sn-Bi-0.5CuZnAl/Cu interface is lower than that of Sn-Bi/Cu inter- can be occurred between Sn-Bi and Cu nanoparticles. With the for-
face. It is found that the CuZnAl memory particles can remarkably mation of Bi balls and Cu clusters surrounded by Cu6Sn5 and Cu3Sn,
suppress the IMC growth of Sn-Bi/Cu interface at 250 °C. Sn-Bi and obtaining high-reliability IMC solder joints. For Sn-Bi solder bear-
Sn-Bi-0.5CuZnAl solders have also been utilized in 3D packaging ing Ni nanoparticles [125], a ternary scallop-shaped (Cu, Ni)-Sn
with transient liquid phase (TLP) bonding [118]. With the addition IMC layer can be formed at the interface. Meanwhile, the Ni
of CuZnAl shape memory particles, the diffusion flux of Cu atoms nanoparticles can reduce the growth of Cu3Sn layer due to the for-
can be decreased, and the growth of IMCs layers is inhibited, the mation of fine Sn-Ni particles. In Sn-35Bi-1Ag solder, 0.5 %Ni
formation of voids is reduced significantly. nanoparticles can hinder the IMC growth due to the change the dif-
fusivity and chemical affinity [126]. The influences of Ti nanoparti-
J RSn58Bi ¼ 3:2J RSn58BiCuZnAl ð22Þ cles as additives on the IMC growth at Sn-Bi/Cu interface was
Sb was added into Sn-58Bi solder, based on EPMA testing [119]. investigated by Jiang [127]. After multiple reflow soldering, the
Only Cu and Sn can be observed across the diffusion reaction layer IMC thickness at Sn-Bi-0.1Ti/Cu interface was distinctly smaller
at the Sn-Bi-Sb/Cu interface. Moreover, the Sb can be found at the than that at Sn-Bi/Cu interface, which further demonstrate that
interface, and the plateaus of Sb and Sn discovered in the diffusion the Ti nanoparticles can suppress the IMC growth.
reaction layer imply that Sb participates at the interface. The In order to improve the interfacial microstructure of Sn-58Bi/
increase of Sb content can increase the total thickness of IMC layer. Cu, Sn-Bi-xLa2O3 (x = 0.1, 0.5, 1.0, 1.5 and 2.0%) solders were pre-
Ga (0.25 to 3.0 wt%) was selected as additives into Sn-Bi solders pared [128]. Compared with Sn-Bi/Cu interface, at Sn-Bi-xLa2O3/
[120]. The Cu9Ga4 IMC layer can instead of the Cu6Sn5 and Cu3Sn Cu interface the IMC grain sizes were significantly smaller. The
phase, and act as a diffusion for the dominant diffusion, which La2O3 nanoparticles can effectively restrain the IMC layer grain
demonstrates that the addition of Ga can suppress the IMC growth. coarsening during the multiple remelting process, and the optimal
Interfacial microstructures of Sn-58Bi solder and Sn-58Bi-0.25Mo content was 0.1%. The reason is that La2O3 nanoparticlesas hetero-
solder on Cu substrate during thermal cycling (35 to 125 °C) were geneous nucleation agent inhibit grain growth. The CeO2 nanopar-
investigated to analyze the effect mechanism of Mo nanoparticles ticles as additives into Sn-Bi solder was investigated by Sharma
Fig. 16. Schematic diagrams of (a) TLPS bonding process and (b) TLPS reactions under various conditions of thermal energy and bonding time [124].
15
Fig. 17. EPMA element mapping of a 0.1 wt% of Ni-MWCNT composite solder [133].
Fig. 18. Sn-Ag-Cu phase diagram: (a) the 240 °C isothermal section of the Sn-Ag-Cu ternary system and (b) Liquidus projection of the Sn-Ag-Cu ternary system [137].
[129]. When the content of CeO2 nanoparticles was up to 0.6%, the 1.02 lm and 0.94 lm. After 1000 h thermal aging, the IMC thick-
IMC thickness at high temperature aging (120 °C, 85% R. H) was ness was 5.12 lm and 4.23 lm, respectively. Ni-decorated
reduced significantly. 0.5 wt% Al2O3 nanoparticles can reduce the NWCNTs were synthesized to analyze the variation of the IMC
IMC thickness at Sn-Bi/Cu interface from 2.5 lm to 1.27 lm after thickness [133], as shown in Fig. 17. Ni and C exhibit a lamellar
aging (288 h, 85 °C) [130]. For the electromigration testing, at structure similar to Sn and Bi. The IMC thickness can be decreased
the cathode, the IMC thickness was reduced by doping Al2O3 obviously after reflow soldering and aging. After 1000 h aging, the
nanoparticles, and the decreasing amplitude was approximately thickness is 4.49 lm and 6.67 lm for Sn-Bi-Ni-MWCNTs/Cu solder
8%. For the Y2O3 nanoparticles [131], the similar suppression joints and Sn-Bi /Cu solder joints, respectively. Lee [134] synthe-
behavior can be found. The author considers that the Y2O3 sized Sn-decorated MWCNTs, and also incorporated into Sn-Bi sol-
nanoparticles can pin the Cu6Sn5 grain boundary resulting in lower der. IMC thickness at Sn-Bi /Cu solder joints was 0.97 lm (after
surface energy of the IMC, to inhibit the IMC growth. reflowing), 1.81 lm (500 h aging), 4.98 lm (1000 h aging). With
Ag-decorated NWCNT was selected as additive into Sn-58Bi sol- the addition of 0.1 wt% Sn-MWCNTs, the thickness can be changed
der [132]. The interfacial reaction between Sn-Bi solder containing to 0.83 lm (after reflowing), 1.45 lm (500 h aging), 4.34 lm
Ag-decorated NWCNT on Cu substrate has been investigated. The (1000 h aging), respectively. The suppression effect can be attribu-
thickness of Cu6Sn5 layer formed at the interface with the addition ted to the interrupt atomic diffusion with the addition of Sn-
of 0 wt% and 0.1 wt% Ag-decorated NWCNT can be calculated to be MWCNTs.
16
2. Microstructure evolutions ture of Sn-Ag-Cu solder alloys. For different constituent Sn-Ag-Cu
solders (Sn-3.9Ag-0.6Cu, Sn-3.5Ag-0.7Cu and Sn-3.0Ag-0.5Cu),
2.1. Sn-Ag-Cu solders the rapidly cooled Sn-Ag-Cu samples exhibited the typical
microstructures are composed of the eutectic phase and b-Sn, in
For lead-free solders, the microstructure of the matrix directly addition. Large primary Ag3Sn platelets can be found in slowly
determines the performance (wettability, mechanical property, cooled Sn-3.9Ag-0.6Cu and Sn-3.5Ag-0.7Cu since the high-Ag
hardness and reliability) of the solder and solder joint [135,136], contents.
and is also an important index to evaluate the solder. For Sn-Ag- Gao [139] considered that the rare earth Nd can modify the
Cu alloys, the microstructure evolution and phase distribution microstructure of Sn-3.8Ag-0.7Cu lead-free alloy. The content of
have been investigated systematically. Sn-Ag-Cu solders with Nd determines the microstructure evolution. With the addition of
reflow soldering, the soldering temperature is generally controlled 0.025 wt% Nd, the refined microstructure can be found compared
at around 240 °C. Fig. 18 shows the phase diagram of Sn-Ag-Cu sol- with original Sn-Ag-Cu solder. Moreover, 0.05% Nd enables the
ders [137]. At 240 °C, considering Sn is the main body of Sn-Ag-Cu microstructures of the Sn-Ag-Cu alloys to be the refined to the
solder and the content of Ag and Cu in trace, Cu6Sn5 and Ag3Sn are maximum extent. Small eutectic particles turn to be more uniform
precipitated from the matrix during the transformation of liquid distributed in the matrix. When the content of Nd increases up to
solder into solid state. At 216 °C (critical temperature), the reaction 0.1%, or more than 0.1%, Sn-Nd IMC particles can be formed with
(L = Cu6Sn5 + Ag3Sn + Sn) can be occurred. After reflow soldering, the reaction between Sn and Nd and observed in the Sn-Ag-Cu sol-
the size and the distribution of Cu6Sn5 and Ag3Sn become the ders, which can induce the deleterious effects on the properties of
investigation focus to determine the properties of solder joints. lead-free solder joints in service. The addition of Pr can signifi-
Kim [138] investigated the effects of cooling speed on microstruc- cantly reduce the supercooling degree required for the solidifica-
Fig. 19. Microstructures of Sn-Ag-Cu and Sn-Ag-Cu-Ce: (a) Matrix of Sn-Ag-Cu; (b) Matrix of Sn-Ag-Cu-Ce; (c) Ag3Sn of Sn-Ag-Cu; (d) Ag3Sn of Sn-Ag-Cu-Ce; (e) Cu6Sn5 of Sn-
Ag-Cu and (f) Cu6Sn5 of Sn-Ag-Cu-Ce [141].
17
tion of Sn-Ag-Cu solders, refining the solder structure, reducing the son for the formation of large Ag3Sn platelets. The addition of Ti
size of primary b-Sn in the solder, and inhibiting the formation of can also modified the microstructures of Sn-3.0Ag-0.5Cu solder
bulk Ag3Sn. However, excessive Pr addition will cause the forma- [143]. With the addition of 0.2 wt% Ti, new IMCs (Ti2Sn3 and (Ti,
tion of Pr3Sn phase inside the solder and reduce the performance Fe, Cu)Sn2) can be formed and observed, and reduce the nucleation
of the solder [140]. For the addition of 0.03 wt% rare earth Ce undercooling for b-Sn in both freestanding solder balls and in
[141], the microstructures of Sn-Ag-Cu can be refined obviously, joints on Ni and Cu substrates. For the addition of Ga, less and finer
as shown in Fig. 19. The size of IMC particles (Ag3Sn and Cu6Sn5) precipitates have formed in the Sn-3.0Ag-0.5Cu solder, which can
can be reduced, especially for the transformation of Ag3Sn phase be attribute the Ga hinder the formation of the secondary phase
from needle-type to spot-type, which further demonstrate the [42]. The addition of Fe into Sn-1.0Ag-0.5Cu can induce the forma-
refinement effect of trace amount of rare earth elements. tion of new IMC, namely FeSn2 phase [144], as shown in Fig. 20.
The synergetic effects of adding 0.1 wt% of Fe, Co, Te and 2 wt% The FeSn2 particles sparsely distribute in the matrix microstructure
Bi into Sn-3.0Ag-0.7Cu solder are investigated by Ei-Taher [142] in existed in the interdendritic areas. The increasing of Fe content can
terms of the growth of large platelets Ag3Sn IMC, which can induce increase the number of FeSn2 particles obviously. Similarly, in Sn-
the formation of SnTe, FeSn2, (Cu, Co)6Sn5 and Bi in the Sn-Ag-Cu 1.0Ag-0.5Cu low-Ag alloy, the addition of Fe can also induce the
alloy with b-Sn, Ag3Sn and Cu6Sn5. The morphology of Ag3Sn can FeSn2, 0.05 wt% Fe and 1 wt% or 2 wt% Bi coupling added into
be changed from large platelets into fine needle-like structure. Sn-1.0Ag-0.5Cu solder [145]. During aging, the partial Fe can solute
Moreover, the volume fraction of Ag3Sn can be decreased obvi- into Sn in the eutectic colony, which can reduce the Ag diffusivities
ously. Since the temperature of the solder is 600 °C in the smelting and in the Cu6Sn5 can decrease the microstructure coarsening rate.
process, relatively high smelting temperature is also the main rea- Bi in the matrix can reduce the Sn activity in the chemical reaction
Fig. 20. Microstructures of Sn-1.0Ag-0.5Cu-xFe solder [144].
18
between Cu and Sn, Ag and Sn. Therefore decrease the amount of particles with network structure in the matrix. Nevertheless the
Ag3Sn and Cu6Sn5 particles. Zn element can also react with matrix Cu6Sn5 dispersed at the eutectic colony uniformly. With the addi-
elements, only with Cu and Ag, not Sn, scallop-like and plate-like tion of Ni nanoparticles, a very fine (Cu, Ni)-Sn particles can be
(Cu, Ag)5Zn8 formed with an average size of 70 lm can be found formed and distributed evenly in the matrix. Compared with Sn-
in the Sn-1.0Ag-0.3Cu matrix [146]. 2.0 wt% Zn addition can Ag-Cu solder, the Ni nanoparticles can reduce the size of Ag3Sn
decrease the volume fraction of Ag3Sn particles and increase the IMC, and impede the growth of Sn grains. For the addition of Mo
inter-particle distance. 3.0% Zn addition can refine the microstruc- nanoparticles [151], the Ag3Sn particles dispersed in the matrix
ture of Sn-Ag-Cu solder, decreasing the average size of (Cu, Ag)5Zn8 are extremely fine compared with the original Sn-3.0Ag-0.5Cu
and inter-particle distance, and increasing the volume fraction of alloy, during aging. The size of Ag3Sn particles are still smaller than
Ag3Sn and (Cu, Ag)5Zn8. 1.0 wt% Zn can also promote the formation that in the Sn-3.0Ag-0.5Cu solder. For the Sn-3.8Ag-0.7Cu solder
of (Cu, Ag)5Zn8 in Sn-3.0Ag-0.5Cu and Sn-1.0Ag-0.5Cu solder [147], bearing CuZnAl particles [67], the number and the area of eutectic
and can inhibit the formation of Ag3Sn plates. High-Ag solder will particles increases greatly. The average distance between arms of
result in the increase of Ag content in (Cu, Ag)5Zn8 phase. In Mao’- the dendrites can be changed from 14.7 lm to 11.3 lm. The CuZ-
work [148], With 0.2% Zn addition into Sn-3.0Ag-0.5Cu solder, no nAl can play a strengthening role in the solder matrix. Adding a
Zn-rich phase can be observed by EDS in the matrix, resulting by small amount of Mn nanoparticles (0.02, 0.05, 0.1 and 0.3 wt%)
the low content of Zn in the solder. 0.2 wt% Sb with Sn tends to can also improve the microstructure of Sn-0.3Ag-0.7Cu solder
form solid solution, meanwhile uniformly distributes in the [152]. Based on EDX testing, it is inferred that the matrix of Sn-
microstructure. 0.2% Mn can react with Sn to form MnSn2 IMC Ag-Cu-0.3Mn include b-Sn, Ag3Sn, Cu6Sn5 and MnSn2. It is obvious
phases randomly dispersed in the Sn-Ag-Cu alloy. The addition of that the addition of Mn nanoparticles can reduce the size of Ag3Sn
Sb, Mn, Zn into Sn-Ag-Cu solders can remarkably refine the eutec- particles and the distance between the particles. The Mn nanopar-
tic microstructure. The coupling addition of Bi and Ni elements into ticles improve the high nucleation density of the second phase in
low-Ag Sn-0.7Ag-0.5Cu solders can significantly cause the matrix the eutectic region during solidification. With the further increase
microstructure to be refiner [149]. of Mn content, in the matrix microstructure, the refinement of b-Sn
Fig. 21 shows the SEM microstructure and elemental analysis of and Ag3Sn particles improved can be observed. Co nanoparticles
Sn-Ag-Cu solder and Sn-Ag-Cu bearing 0.5% Ni (20–35 lm in diam- can also react with Sn, forming (Cu,Co)6Sn5 and (Co,Cu)3Sn. These
eters) nanoparticles [150]. It is found that the needle-typed Ag3Sn particles with Ag3Sn homogeneously distributed in the matrix
Fig. 21. SEM microstructures of solders: (a) Sn-Ag-Cu; (b) Sn-Ag-Cu-0.5Ni; (c) Elemental analysis as marked ‘‘P” in Sn-Ag-Cu and (d) Elemental analysis as marked ‘‘Q” in Sn-
Ag-Cu-0.5Ni [150].
19
[153]. The microstructure of Sn-Ag-Cu-0.8Co solder shows a uni- matrixes surrounded by the eutectic network region consisting of
form distribution of very fine other phases in the b-Sn matrix. FeCo Cu6Sn5 and Ag3Sn particles can be observed in the Sn-Ag-Cu and
magnetic nanoparticles were utilized as additives into Sn-3.0Ag- Sn-Ag-Cu-CNT solders. With the increase of MWCNT content, the
0.5Cu solder [154]. Based on TEM observation, no Co react with grain size of b-Sn matrixes gradually decreases, which can be
Sn to form IMC. FeCo nanoparticles are distributed in the b-Sn attributed to the inhibition coarsening effect of MWCNT. Dual cera-
matrix as heterogeneous nucleation sites. With the increase of mic nano-materials (TiO2 and graphene) were considered as addi-
FeCo content, the amount of Ag3Sn and b-Sn dendrites can be tives into Sn-3.0Ag-0.5Cu solder [158]. Fig. 22 shows the
reduced obviously. The addition of Al nanoparticles can affect the microstructures of Sn-Ag-Cu and Sn-Ag-Cu bearing TiO2 and gra-
microstructure of Sn-3.8Ag-0.7Cu solder [155,156]. The results phene. Different size of b-Sn grains can be observed. For Sn-Ag-
demonstrate the Al nanoparticles can decrease the average size Cu, Sn-Ag-Cu-0.03% (TiO2 and graphene), Sn-Ag-Cu-0.12% (TiO2
of the Cu6Sn5 and Ag3Sn particles, and the distance between parti- and graphene), Sn-Ag-Cu-0.21%(TiO2 and graphene), Sn-Ag-Cu-
cles remarkably. The microstructures of solder bearing Al nanopar- 0.6% (TiO2 and graphene), Sn-Ag-Cu-0.21% (TiO2) solders, the b-
ticles become finer. The nanoparticles can be found using TEM Sn area are approximately 635.87 lm2, 512.82 lm2, 406.05 lm2,
testing, and the nanoparticles tend to be located at the grain 315.0 lm2, 478.79 lm2, 373.22 lm2, respectively, which indicates
boundaries in the b-Sn matrix, which will enhance the creep per- that the addition of TiO2 and graphene can reduce the b-Sn size.
formance of solder. Meanwhile, the optimal concentration of 0.21% (TiO2 and gra-
MWCNT can also modify the microstructure of Sn-3.0Ag-0.5Cu phene) can be demonstrated, indicating that the addition of TiO2
solder [157]. Microstructural analysis clearly indicated that b-Sn and graphene has a remarkable effect in refining the b-Sn grains
Fig. 22. Microstructures of solders: (a) Sn-Ag-Cu; (b) Sn-Ag-Cu-0.03% (TiO2 and graphene); (c) Sn-Ag-Cu-0.12% (TiO2 and graphene); (d) Sn-Ag-Cu-0.21% (TiO2 and graphene);
(e) Sn-Ag-Cu-0.6% (TiO2 and graphene) and (f) Sn-Ag-Cu-0.21% (TiO2) [158].
20
of Sn-Ag-Cu solders. The authors consider this phenomena can be reduced significantly, which demonstrates the retardation effect of
attributed to the adsorption of nano-materials on the b-Sn grain the ZnO nanoparticles. The effect of La2O3 nanoparticles on the
in the matrix. 0.5 wt% Al2O3 nanoparticles were selected to prepare microstructure of Sn-3.0Ag-0.5Cu solder was investigated by
Sn-3.0Ag-0.7Cu composite solders [159]. The average size of Ag3Sn Sharma [163]. Based on SEM observation, when the content of
phase was about 0.95 lm. With the addition of Al2O3 nanoparti- La2O3 nanoparticles is more than 0.5 wt%, the microstructure with
cles, the size of Ag3Sn particles can be changed about 0.36 lm. refined grains can be found, which indicates that the La2O3
Moreover, the eutectic bands can be changed wider, so the investi- nanoparticles can reduce grains size. The growth inhibition of grain
gation further demonstrate that the addition of nanoparticles can size and IMCs can be attributed to the adsorption of La2O3
refine the size of Ag3Sn phase. The reason is Al2O3 nanoparticles nanoparticles in the matrix. AlN nanoparticles was selected as
promote a high nucleation density of the second phase in the additives into Sn-3.0Ag-0.5Cu solder to enhance the microstruc-
eutectic colony during solidification. SnO2 nanoparticles reinforced ture and properties [164]. Different weight contents of AlN (0,
composite Sn-3.0Ag-0.5Cu solder fabricated by accumulative roll- 0.03, 0.12, 0.21, 0.60 wt%) were incorporated into Sn-3.0Ag-0.5Cu
bonding process was investigated by Anattiya [160]. The solders. The AlN particles can refine the grains in the matrix, and
microstructure of the Sn-Ag-Cu solder bearing SnO2 nanoparticles the average area of b-Sn can be reduced significantly. The optimal
was composed of b-Sn phase and eutectic phase. The eutectic content of AlN nanoparticles was demonstrated to be 0.21 wt%, the
phase was elongated in the roll direction. due to the addition of average area of b-Sn in Sn-Ag-Cu solder can be decreased from
SnO2 particles, the microstructure was finer and higher 688.31 lm2 to 363.16 lm2 by adding 0.21 wt% AlN. However, with
homogeneity. the addition of 0.60 wt% AlN nanoparticles, due to the higher sur-
The addition of ZrO2 nanoparticles can also affect the face energy of nanoparticles, the excessive content of AlN nanopar-
microstructure of Sn-Ag-Cu solder. The Sn-3.0Ag-0.5Cu solder ticles can form agglomerates, which can induce the coarsening of
bearing ZrO2 on Au/Ni metallized Cu pads was investigated by Gain microstructure compared with Sn-Ag-Cu solder bearing 0.21 wt%
[161]. In the b-Sn matrix, Ag3Sn, Cu6Sn5, AuSn4 and ZrO2 particles AlN nanoparticles. Fig. 23 shows the TEM microstructures of Sn-
can be found to be uniformly distributed. The existence of sec- Ag-Cu-0.12AlN and Sn-Ag-Cu-0.21AlN solders. The AlN particles
ondary particles can improve the strength of solder joints. But in embedded in the matrix can be observed. The AlN nanoparticles
the work, no report about the effect of ZrO2 on the b-Sn matrix. are adsorbed on the Ag3Sn, Cu6Sn5 and the b-Sn grains, so their
ZnO nanoparticles were added into Sn-3.5Ag-0.5Cu solder [162], growth can be restricted. NiO nanoparticles can also reduce the
the grain sizes and b-Sn interdendritic arms and IMC particles were grain sizes of the solder. High viscous solder performance
Fig. 23. Dark-field TEM: (a) Sn-Ag-Cu; (b) Sn-Ag-Cu-0.12AlN; (c) Sn-Ag-Cu-0.21AlN and (d) TEM-EDS mapping of (c) [164].
21
restricted grain kinetics until nanoparticles were unpinned from Bi as additive into Sn-3.5Ag can refine the microstructure [172].
the matrix during reflow soldering [58]. Sn-1.0Ag-0.5Cu reinforced In the Sn-3.5Ag solder, the primary b-Sn phase and eutectic struc-
with SiC nanoparticles was investigated by EI-Daly [165]. With the ture including Ag3Sn IMC and b-Sn phase, with 0.3 wt% Bi addition,
addition of 0.35 wt% SiC, the average size of b-Sn grains can be the primary b-Sn phase and eutectic structure can be refined
changed from 80.0 ± 3.5 lm to 50.0 ± 3.5 lm, which shows that remarkably. The content of primary b-Sn phase decreases and the
the SiC nanoparticles can refine the microstructure (b-Sn and IMCs) Ag3Sn IMC are embedded in the matrix uniformly to form a fine
of solder. But 0.75 wt% SiC can decrease the volume fraction of eutectic structure. So the addition of Bi can hinder the formation
IMCs particles and increase the inter-particle spacing. For TiC of primary b-Sn phase. Meanwhile, Bi does not react with Sn and
nanoparticles in Sn-3.0Ag-0.5Cu solder [166]. The refinement Ag to form IMC particles in the matrix, and the solid solubility of
effect can be also verified, and the adsorption of TiC nanoparticles Bi in the Sn matrix is very few. So Bi mainly exists in the form of
can lower the growth of Ag3Sn. During aging, the positive effect of elements. Eq. (23) and Eq. (24) can be used to calculate the critical
TiC nanoparticles can be demonstrated. In Zhao’work [167], 20 nm nucleation radius and critical nucleation energy using classical
Fe2O3 nanoparticles can effectively refined the b-Sn grains. When nucleation theory. At the solid-liquid interface Bi segregation can
the 50 nm and 200 nm Fe2O3 nanoparticles were added, the size induce the reduction of solid-liquid interface tension, which will
of b-Sn grains can be increased compared with that with 20 nm decrease the critical nucleation radius and critical nucleation
Fe2O3 nanoparticles added, which further illustrates that the size energy. It is imperative to enhance the more crystal nucleus and
of Fe2O3 nanoparticles is the critical factor to refinement effect. a refined eutectic structure. The effect of Cr (1, 3 and 5 wt%) on
SrTiO3 nanoparticles were added into Sn-3.0Ag-0.5Cu solder on the microstructure of Sn-3.5Ag solder was investigated by Gumaan
Au/Ni metallized Cu pads, and can refine the AuSn4, Ag3Sn, Cu6Sn5 [173]. The addition of Cr element did not react with the matrix ele-
in the matrix [168]. SrTiO3 nanoparticles can reduce the size of b- ment Sn or Ag to form IMCs. The XRD demonstrates that the partial
Sn grains from 10 to 15 lm to 7–10 lm. Cr dissolve into Sn matrix, and undissolving Cr atoms have precip-
itated as Cr phase in the Sn-Ag matrix. The results indicated that
the Cr content can refine the microstructures of Sn solders matrix,
2.2. Sn-Ag solders suppressing coarse IMC formation, and changing the IMC morphol-
ogy in solder. Ti is the active transition metal, can be added into Sn-
Among series of environmental-friendly lead-free solders as 1.0Ag solder [174]. New Ti2Sn3 phase and SnAgTi eutectic in the
electronic interconnect materials in electronic packaging, the Sn- matrix microstructures can be observed, respectively, which can
Ag binary solders with good wettability on different substrates decrease the size of b-Sn grains. Ti2Sn3 will form prior to the solid-
and good properties (mechanical properties and thermal fatigue ification of Sn-Ag-Ti, and move to the bottom part, being jostled to
resistance) are considered as one of the promising candidate mate- b-Sn grain boundaries or dendrite cell boundaries. With 0.27 wt%
rials to replace the traditional Sn-Pb solders [9,169]. Therefore, the Ti adding into Sn-3.5Ag solder, the grain boundaries became
investigation of microstructures and properties of Sn-Ag solder thicker. with 0.27 wt% Cd can refine the b-Sn grain, and some
become the more important role in electronic field. Moreover, agglomeration can be found in the microstructure [175]. The addi-
Sn-3.5Ag has been utilized in 3D packaging for high quality wafer tion of Ni can influence strongly the solidification microstructure
bonding [170]. After long time reflow and aging, the complete IMC of the matrix [176]. The size of b-Sn grain can be reduced. The
solder joints can realize the 3D stacking, which demonstrates the author consider the Ag3Sn, Ni3Sn4, Ni, NiO and Ag phases dispersed
utilization of Sn-3.5Ag solder as interconnection materials. The in the matrix, but no XRD testing was not show to support the
Sn-Ag binary phase diagram is shown in Fig. 24 [171]. Sn-3.5Ag conclusion.
is the eutectic composition consisting of b-Sn phase and Ag3Sn par-
ticles in the matrix microstructure. The mutual solubility of Ag and 2rLS
r ¼ ð23Þ
Sn is very low, and two elements can react to form Ag3Sn phase. It DGm
has been found in a large number of literature that the Ag3Sn phase
mostly exists in the matrix with needle-like morphology. In order 3
16 r
to improve the microstructure and performance of Sn-Ag solder, DG ¼ p LS ð24Þ
3 DG m
some other elements and particles such as Cu, Ni, CNT are usually
added to modify the properties. where rLS is the solid-liquid interface tension; DGm is the Gibbs free
energy difference between liquid and solid per unit volume.
For Sn-3.5Ag solder, three different sizes of Cu particles (20–
30 nm, 3 lm and 15 lm) were chosen for modifying of microstruc-
ture [177]. With the addition of Cu nanoparticles, the b-Sn grains
refinement with more dispersed Ag3Sn/Sn mixture can be found.
The Cu nanoparticles can reduce the dendrite arm spacing. The
microstructure of Sn-3.5Ag doping microparticles was not as
strong as found in the solder doping nanoparticles. The sunflower
morphology of un-dissolved Cu can be found in the solder bearing
microparticles, which was consisted of petal region (Cu6Sn5) and
pure Cu. In order to modify the size of Ag3Sn phase, changing of
the conent of Ag in the Sn-Ag solder may be also an effective
way. Fig. 25 shows the microstructures of Sn-xAg solder [178]. In
Sn-3.0Ag and Sn-3.5Ag, b-Sn was surrounded by fine lamellar net-
works. While large plate-like Ag3Sn IMC was found in Sn-4.0Ag and
Sn-4.5Ag. Moreover, the increase of Ag content can increase the
area fractions of eutectic and primary Ag3Sn. So the decrease of
Ag3Sn can refine obviously the microstructure of solder. Niranjani
[179] selected 1.5 wt% Mo and 1.5 wt% Ni nanoparticles to affect
Fig. 24. Binary phase diagram of Sn-Ag system [171]. the microstructure of Sn-3.5Ag solder, but the author did not find
22
Fig. 25. Microstructures of Sn-xAg solders [178].
the changes of b-Sn grains and the Ag3Sn distribution with the decreased by a few micrometers due to the ball milling energy.
addition of Mo or Ni nanoparticles using SEM but the uniform dis- After 6 h of ball milling, only a small portion of the solder surface
tribution of nanoparticles in matrix using TEM, which maybe the had embedded CNTs. After 24 h of ball milling, the embedded CNTs
excessive nanoparticles addition reduce the positive effect on the covered the entire surface of the solder balls. Cu-coated CNTs as
refinement of microstructure. In Xia’s work [180], with the addi- additives can influence the microstructure of Sn-3.5Ag solder
tion of Cu and Ni microparticles with a volume fraction of 5%, [183]. The dendritic arm spacing and Ag3Sn IMC can be reduced
the microstructure of Sn-3.5Ag solder was remarkably improved. obviously. The Cu-CNTs with high surface energy can increase
After reflow soldering, there are obvious IMCs formed around the the number of heterogeneous nucleation centers, which will
microparticles, and the central region of the microparticles is still induce the reduction of secondary dendrite arm spacing and
Cu or Ni metal, which forms a sunflower shape particles in the refinement of microstructure. 0.3 wt% ZnO nanoparticles were
matrix, strengthing the solder. Cu and Sn microparticles are simul- selected to be added into Sn-3.5Ag solder. The results revealed that
taneously added into Sn-3.5Ag solder in a certain proportion [181], the grain size of b-Sn is seen relatively smaller than that in original
and Cu6Sn5 particles are completely formed in the molten solder to Sn-Ag solder, which shows the refinement effect of ZnO nanoparti-
enhance the properties of solder joints. cles in Sn-Ag solder [184]. Sn-Ag solder containing CeO2 nanopar-
Surface impact mixing process was utilized to investigate the ticles have been pulse electrodeposited from an aqueous citrate
Sn-3.5Ag solder ball incorporated with CNTs [182]. The BGA sam- bath [185]. With the increase of CeO2 content, the finer microstruc-
ple after reflow with 245 °C for 20 s as shown in Fig. 26. During sur- ture of the deposits can be observed, and the grains size is reduced
face impact mixing process, the length of the CNTs can be remarkably. The authors suggest that the phenomena can be
Fig. 26. Sn-Ag incorporated CNTs solder balls: (a) Low magnification and (b) high magnification [182].
23
Fig. 27 shows the Sn-Cu phase diagram [188]. Only 0.006 wt% or
0.01% Cu can be dissolved into Sn at eutectic temperature. The
reaction between Sn and Cu can be found to form IMCs with the
variation of Cu content, and the eutectic reaction can be demon-
strated as the equation (Liquid ? b-Sn + Cu6Sn5) at 227 °C. The
eutectic Sn-0.7Cu solder has been proposed as the good alloy to
replace traditional Sn-Pb solder due to the low cost and the good
properties.
The rare earth Ce as additives into Sn-0.7Cu solder can modify
the microstructure [189]. With the addition of Ce, two different
new particles (CexOy and CeSn3) can be observed in the Sn-Cu
matrix, and the smaller eutectic microstructure can be demon-
strated. But excessive Ce can lead to the coarsening of the
microstructure due to formation of bulk phase particles containing
Ce. In Zhang’s work [190], it is further proved that the addition of
rare earth Ce should be controlled in trace amount. Small amount
of rare earth Ce can refine the microstructure of solder. For Sn-
0.7Cu-0.05Ni-xPr alloys [191], the microstructural refinement of
the matrix can also be observed with the addition of Pr. Compared
Fig. 27. Sn-Cu phase diagram [188].
to the Sn-Cu-Ni original solder, Pr can prevail the more uniform
microstructure and reduction of b-Sn grains. Moreover, the optimal
attributed to the nucleation centers of CeO2 particles and the content of Pr has been demonstrated to be 0.05 wt%. Rare earth Eu
increasing cathodic polarization of CeO2 adsorption on the cathode present similar modify effect in Sn-0.7Cu-0.05Ni alloy [192]. The
surface. POSS particles were selected as additives into Sn-3.5Ag reaction between Sn and Eu can be occurred to be EuSn3 phase.
solder [186]. POSS can decease the average size of IMCs and the Small EuSn3 particles can be found to existed in the boundaries
spacing between them effectively. By optimizing design, 3.0 wt% of b-Sn grains, and the second particles act as obstacles to pin dis-
POSS can refine the microstructure of the solder to the maximum location, which will induce the increase of applied stress required
extent. to move dislocation.
In order to develop lead-free solders suitable for automotive use
2.3. Sn-Cu solders instead of conventional Sn-Pb alloy due to the environmental reg-
ulations, Koo [193] investigated the Sn-0.5Cu solder with the addi-
Sn-Cu lead-free solder is one of the most widely used in elec- tion of Al. The small amount of Al addition can remarkably change
tronics industry, which has been utilized extensively in wave sol- the microstructure of Sn-Cu solder. With the increase of Al content
dering [187]. The phase distribution and microstructure (0.03–0.05 wt%), eutectic b-Sn + Cu6Sn5 IMC networks can be
evolution of Sn-Cu solder are the important roles in electronic refined effectively. Based on TEM testing, it is demonstrated that
industry, because the microstructure of solder directly determines the Cu will react with Al to form Cu-Al IMC, as shown in Fig. 28.
the properties of solder and solder joints. In Sn-Cu alloy system, The authors consider the Cu-Al IMC is d-Cu33Al17. For the addition
Fig. 28. TEM microstructure of Sn-0.5Cu-0.05Al: (a) overall TEM of Sn-0.5Cu-0.05Al; (b) magnified TEM of Cu-Al IMC and (c) magnified TEM of grain boundary [193].
24
of 0.2 wt% Cr, Cr can also react with Sn in Sn-0.7Cu solder to form location and hinders the b-Sn grain growth. SiC nanoparticles
CrSn2 IMC [194]. The EPMA testing demonstrated that the CrSn2 have been attempted to affect the microstructure of Sn-0.7Cu
IMC can uniformly distribute in the Sn-Cu-Cr matrix to reduce alloy [204]. With the addition of 2.0 wt% nanoparticles, there is
the grains size. Ni was added into Sn-0.7Cu solder by Silva [195]. no obvious refinement effect on the matrix microstructure of
The (Cu, Ni)6Sn5 IMC can be formed both in the eutectic and as a the solder, and random distributions of SiC can be found. In addi-
primary phase. Ni3Sn4 IMC can also be observed with needle- tion, clustering of SiC particles can be observed in the matrix,
type morphology. (Cu, Ni)6Sn5 IMC and Ni3Sn4 IMC can be found resulting in agglomeration and segregation of SiC particles due
for the early positions in the directional solidification castings to the van der Waals forces, but the further SEM and TEM need
obtained for Sn-Cu-Ni solder. EI-Daly [196] selected Ag and In as to investigate the effect of SiC nanoparticles on the microstruc-
additives into Sn-0.7Cu alloy. The microstructure of Sn-Cu solder ture of Sn-Cu solder. In EI-Rehim’s work [205], Cu6Sn5 and Cu10-
consists of b-Sn phase and Cu6Sn5 phase. With the addition of Sn3 can be found in Sn-0.7Cu solder. With the addition of ZnO
2.0 wt% Ag, many fiber-type Ag3Sn phases can be observed. The nanoparticles, the average sizes of both IMCs are reduced obvi-
author considers that the fiber-type Ag3Sn IMCs can pin the grain ously. 0.25 wt% ZnO nanoparticles can refine the microstructure
boundaries in the alloy, stabilizing and refining the matrix of Sn-Cu solder. Nanoparticles tend to concentrate on the surface
microstructure of solder. In as additive into Sn-Cu solder can of IMC particles, thus reduce the growth of IMC. Salleh [206]
induce similar microstructure, suppressing the formation of large demonstrated that the TiO2 nanoparticles existed on the Cu6Sn5
b-Sn dendrite. Due to the higher activity of In, the formation of surface. Adsorption effect of nanoparticles can improve the
SnIn4 IMC can be demonstrated in the matrix, which can retrain microstructure and properties of Sn-0.7Cu solder.
the formation of Cu6Sn5 IMC. The effect of S on the microstructure
of Sn-0.7Cu solder was investigated [197]. It clears that the addi- 2.4. Sn-Zn solders
tion of S into Sn-Cu solder makes the intensity of Sn3O(OH)2Cl2
phase obvious than the original Sn-Cu alloy. The experimental Among binary lead-free alloys, the melting point of Sn-9Zn sol-
results demonstrate that the Sn-Cu-S solder has better corrosion der is closest to traditional eutectic Sn-Pb alloy [207,208], this
resistance than the Sn-Cu solder. The addition of In into Sn- means that if Sn-Zn is selected for soldering in electronic industry,
0.7Cu-0.2Ni solder can slow down the corrosion of the surface, the soldering process parameters are basically close to the Sn-Pb
which represents that the addition of In can increase the corrosion solder. On the earth, Zn is abundant, inexpensive and no toxic,
resistance [198]. In the OM microstructure, the element of In can which induces the widely application and research of Sn-Zn alloy,
refine the matrix microstructure. With the addition of Bi into Sn- Fig. 30 shows the Sn-Zn phase diagram.
0.7Cu solder [199], the Cu6Sn5 fiber and diameter of Sn-Cu solder The microstructures of Sn-9Zn solder consists of gray b-Sn
can be reduced with the increase of Bi content after directional phase and black needle-like Zn-rich phase, the Zn-rich phase is
solidification, which can be attributed to the restriction of disloca- random distributed in the b-Sn matrix, with a length of up to hun-
tion slip, grain boundary, solid solution precipitated. The solid dreds of micros and a width of only 3–6 lm. With the addition of
solution containing Bi can nucleation site for the Cu6Sn5 fiber rare earth Pr (0.01–0.08 wt%), the size of Zn-rich phase in the sol-
and reduce the fiber spacing and diameter. In Kanlayasir’s work der can be decreased with the increase of Pr content, and distribute
[200], Ag, Bi, In and Sb were selected to be added into Sn-0.6Cu- more uniformly in the matrix [209]. When the content of Pr is
0.05Ni-Ge solder. Ag addition can increase the size of b-Sn grains. 0.08 wt%, the rare earth phase containing Pr is found in the matrix,
Bi, In and Sb can decrease the b-Sn grains size. Only OM tests were which is determined to be PrSn3 by EDS. The rare earth elements
used in this study, the SEM and the elemental analysis are needed have stronger Sn affinity, therefore, rare earth elements are impor-
for the further study. tant elements in the alloying of lead-free solders. Moreover, rare
Ni microparticles as additives can also modify the microstruc- earth Er [210], La [211] and Y [212] have been proposed as addi-
ture of Sn-0.7Cu solder [201], due to the small atomic diameter tives into Sn-9Zn solder, the microstructure of Sn-Zn-0.08Er, Sn-
difference and face-centered cubic crystal structure between Cu Zn-0.06La and Sn-Zn-0.06Y are much finer than that of original
and Ni, trace amount of Ni microparticles can induce the forma- Sn-Zn solder, especially for the reduction of Zn-rich phases in the
tion of (Cu, Ni)6Sn5 phase, when the Ni particles is 0.05 wt%, matrix, excessive rare earth elements will lead to the formation
the IMCs in the matrix are refined and distributed more uni- of ErSn3, LaSn3 and YSn3, bulk rare earth phase will degrade the
formly, however, with the increasing of Ni content further, coars- properties of solder joints in service. Rare earth Nd also was added
ening (Cu, Ni)6Sn5 phase can be found. Sn-0.7Cu solders doping into Sn-9Zn solder [213], the size of needle-like Zn-rich phase can
with different content of graphene nanosheets (GNSs) were inves- be reduced to obtain a uniform and fine microstructure, moreover,
tigated to determine the effect mechanism [202], Fig. 29 shows when the content of Nd is 0.1 wt%, the NdSn3 phases can be
the microstructures of Sn-0.7Cu solders bearing GNSs, when the observed.
content of GNSs is more than 0.025 wt%, the flake GNSs can be EI-Daly [214] investigated the effect of Ni and Sb on the
observed at grain boundary of composite alloy, when the content microstructure of Sn-6.5Zn solder, Ni as additive can refine the
of GNSs is more than 0.075 wt%, GNSs tend to accumulate which microstructure and form particulate flower-shape (Ni,Zn)3Sn4
causes the density of GNSs distributed on the surface of the spec- IMC in the matrix, 0.5 wt% Ni presents a much finer Zn-rich with
imen to increase. Meanwhile, the addition of GNSs, the average small spacing than the original Sn-6.5Zn alloy, however, the Sb
grain size decreased from 35 lm to 25 lm, 17 lm, and 13 lm. can enhance the solid solution effect and increase the refined
But the average grain size increased to about 30 lm for Sn- eutectic area, the Zn-rich can be broken enormously and their
0.7Cu-0.1GNSs, the microstructure become more uniform and shape transforms from needle-type to round-type. With the addi-
finer than the original Sn-Cu solder, the grain boundary migration tion of Bi, the different modified effect can be obtained, the size
of the recrystallized grains id hindered by the diffusely dis- of needle-type Zn-rich can be increased with the increase of Bi con-
tributed GNSs. Si3N4 particles (less than45 lm) can also modify tent, meanwhile, increasing Bi content will induce the small spher-
the microstructure of Sn-0.7Cu solder [203], with the addition oids Bi-rich phase [215].Trace amount of In is added into Sn-9Zn
of Si3N4 particles into Sn-Cu solder, the size of b-Sn grains and solder to analyze the microstructure of Sn-Zn-xIn solder, Fig. 31
the Cu6Sn5 IMC can be reduced greatly, moreover, Si3N4 particles shows the microstructures of Sn-Zn-xIn solders [216], with the
observed using SEM were well distributed between the grain increasing of In content, the concentration and quantity of
boundaries, which will tend to fix the grains preventing from dis- needle-shaped Zn-rich phases can be decreased, and the length
25
Fig. 29. Microstructures of Sn-Cu-xGNSs: (a) Sn-0.7Cu; (b) and (c) Sn-0.7Cu-0.025GNSs; (d) and I Sn-0.7Cu-0.05GNSs; (f) and (g) Sn-0.7Cu-0.075GNSs; (h) and (i) Sn-0.7Cu-
0.1GNSs [202].
of Zn-rich phases can be increased remarkably. Ag and Cu as addi- the Sn-9Zn-1.5Ag-0.7Cu matrix, the authors deem that more con-
tives can also influence the microstructure of Sn-9Zn lead-free sol- sumption of Zn and Sn will cause the weak interface with the orig-
ders [217], with the addition of 1.5 wt% Ag, the fine needle-like Zn- inal matrix. Eq. (25) and Eq. (26) show the cooling reaction for Sn-
rich can be found, dendrite-like dark grey phases (AgZn, Ag5Zn8 Zn-1.5Ag solder and Sn-Zn-0.5Cu solder.
and AgZn3) can be determined with XRD analysis.0.7 wt% Cu can LðliquidÞ ! ðL þ c Ag 5 Zn8 Þ
also refine the Zn-rich phase, the flower or rod-like dark grey
! ðL þ c Ag 5 Zn8 þ e AgZn3 þ AgZn þ b SnÞ
phases (Cu6Sn5, Cu5Zn8 and CuZn5) are precipitated from the Sn-
Zn-Cu matrix. However, dual addition of Ag and Cu into Sn-Zn sol- ! ðc Ag 5 Zn8 þ eAgZn3 þ AgZn þ b Sn
der, large number of Cu-Sn, Ag-Zn and Cu-Zn IMCs can be found in þeutecticb Sn=a ZnÞ ð25Þ
26
decrease the size of primary Zn phase significantly and refine the

eutectic phase [220], moreover, the Cr will react with Sn or Zn to
form Cr2Sn3 and Zn17Cr IMCs. The microstructure evolution of
Sn-9Zn solder with the addition of Na was investigated by Gancarz
[221], with the addition of Na, the size of Zn-rich phase can be
reduced, Zn-rich phase begin to fragment, for Sn-Zn-3.0Na, NaSn,
Na15Sn4 and NaZn13 IMCs can be observed using TEM, as shown
in Fig. 32. By adding 0.05 wt% Ti, a much more homogenous eutec-
tic structure of Sn-9Zn solder can be found obviously [222], nota-
bly, Zn-rich can be refined in the matrix, it is well know that the
refined Zn-rich phase can improve the properties of solder joints,
in addition, by adding a trace amount of Ti can enhance the corro-
sion resistance of Sn-Zn solder significantly. Ga as additive can
improve the microstructure of Sn-8.55Zn-0.5Ag solder [223],
1.0 wt% Ga can induce a less uniform more complicated
microstructure, Sn-8.55Zn-0.5Ag solder with the addition of
2.0 wt% Ga or 3.0 wt% Ga, a coarser and non-uniform microstruc-
Fig. 30. Sn-Zn phase diagram [208]. ture can be observed, AgZn3 is the only IMC in the matrix, Ga can
dissolve in the Zn-rich and Sn-rich phases.
Ag nanoparticles were selected as additives to enhance the
LðliquidÞ ! ðL þ c Cu5 Zn8 Þ microstructure of Sn-9Zn alloy [224]. Ag nanoparticles act as the
! ðL þ c Cu5 Zn8 þ e CuZn5 þ Cu6 Sn5 Þ heterogeneous nucleation sits for the Zn-rich phases, so with the
addition of Ag nanoparticles, the Zn-rich phases become finer
! ðL þ c Cu5 Zn8 þ eCuZn5 þ b SnÞ
and the Ag3Zn IMC particles increases. The results are different
! ðc Cu5 Zn8 þ e CuZn5 þ Cu6 Sn5 þ b Sn with Sn-9Zn bearing Ag element [217]. Different phases can be
þ eutecticb Sn=a ZnÞ ð26Þ found. Sb nanoparticles with different contents were added into
Sn-9Zn solder by Shafiq [225]. For the Sn-Zn-xSb solder, acicular
In addition, in Grobelny’s work [218], the addition of Cu into Sn- shaped Zn-rich phase were homogeneously distributed in the
9Zn solder can increase the corrosion resistance due to the reduc- matrix. Due to the reaction between Sb nanoparticles and Zn
tion of the amount Zn-rich precipitates. Al and Sb were added into phase, the Sb3Zn4 IMC can be clearly observed. Meanwhile, the
Sn-9Zn solder [219], and refined Zn-rich phase and Al6Zn3Sn IMC Sb nanoparticles can reduce the size of Zn-rich phase. This IMC
can be found, the Sb effect was similar with EI-Daly’s work [214], phase results are different with Sn-9Zn bearing Sb element [214],
when the content of Sb is 1.5 wt%, the SbSn IMC can be demon- which may be attributed to the different doping method. After
strated in the matrix. In Sn-8Zn-3Bi solder, Cr as additive can the addition of 3.0 wt% Al2O3 nanoparticles into Sn-9Zn alloy
Fig. 31. Microstructures of Sn-Zn-xIn solder: (a) Sn-Zn; (b) Sn-Zn-0.5In; (c) Sn-Zn-1In and (d) Sn-Zn-2In [216].
27
Fig. 32. TEM microstructure of Sn-Zn-3.0Na solder: (a) NaSn; (b) NaSn; (c) Na15Sn4 and (d) NaZn13 [221].
[226], it is demonstrated that the very fine acicular-shaped Zn-rich [227], which can refine the grains and inhibit the growth of coarse
phase can be observed compared with the microstructure of orig- dendrite Sn-Zn eutectic structure. For Sharma’work [228], with the
inal Sn-Zn solder. Al2O3 nanoparticles can promote a high nucle- addition of CeO2 nanoparticles, needle-like Zn-rich phases are uni-
ation density, which induce the inhibition of the Zn-rich phase formly dispersed in the matrix and have a more regular spheroidal
growth. In ultrasonic semi-solid soldering, Al2O3 nanoparticles shape. The refinement of microstructure can be observed
and Al2O3 microparticles can also represent the refinement effect obviously.
28
2.5. Sn-Bi solders induce the decrease of Bi-rich phase, and the formation of spherical
primary Sn-rich phase. For Sn-58Bi-2.0In and Sn-58Bi-3.0In sol-
Sn-Bi lead-free solder is one of the promising lead-free alloy to ders, the region of Sn-rich extends obviously. Moreover, for the
replace the conventional Sn-Pb solder on account of the low melt- addition of 4.0 wt% or 5.0 wt% In, the new BiIn IMC can be formed
ing temperature [229]. Fig. 33 shows the Sn-Bi phase diagram and observed except for the eutectic Sn-Bi and the primary Sn-rich
[230]. The eutectic composition of Sn-Bi solder is Sn-58Bi, and phase. Ti was added into Sn-58Bi solder [240], and react with Sn to
the low melting point can reduce the risk of the thermal destroy form Ti2Sn3 and Ti6Sn5 IMCs. During thermal aging, these IMCs
to promote the application of Sn-Bi solder [231,232]. The typical keep with the plain morphologies, stabilizing the grain structure
microstructure of Sn-Bi solder is a typical lamellar eutectic struc- of matrix. With the addition of Ti, the solder containing Ti exhibits
ture consisting of alternate-layered Bi-rich phase and b-Sn phase. a considerably refined microstructure compared with the original
For the investigation of Sn-58Bi and Sn-58Bi-1Ag solders [233], Sn-Bi solder. The microstructures of the Sn-58Bi, Sn-40Bi-0.1Cu
more refined microstructure can be found in Sn-Bi-Ag solder com- and Sn-40Bi-2Zn-0.1Cu alloys were studied by Shen [241]. Cu addi-
pared with Sn-Bi solder. The Bi-rich phase can be remarkably tion can refine the grain size of Bi-rich phase in Sn-Bi solder. The
refined and uniformly distributed in the matrix with the addition morphology of Bi-rich shifts from rod-type to spherical or irregular
of 1.0 wt% Ag. Moreover, Ag6.7Sn IMCs were formed during the morphology. Cu can react with Sn to form Cu6Sn5 particles with a
rapid solidification. In Sn-58Bi eutectic solder, the bulk Sn-rich diameter about 4 lm. Bi atoms can segregate and accumulate at
dendritic structure in the matrix can be observed. Rare earth Y the surface of Cu6Sn5 particles. For Sn-40Bi-2Zn-0.1Cu solder, Cu
[234] and Ce [235] elements can refine the microstructure with will react with Zn to form CuZn2 and Cu5Zn8 IMCs, and the remnant
the reduction of Sn-rich and Bi-rich phases. When the content of Zn atoms fathers to form Zn-rich phase during solidification. The
rare earth Y is 0.5 wt%, the bulk dendrite structure can be changed CuZnAl microparticles can also improve the microstructure of Sn-
to spherical morphology. When Al element (0.3, 0.5 and 1.0 wt%) 58Bi solder [242], but excessive CuZnAl will degrade the refining
was added into Sn-30Bi solder [236], it is found that Al can easily effect.
distribute in the Bi-rich phase grain boundary. The eutectic region Ag nanoparticles as additives can modify the microstructure of
can be significantly reduced, and Bi-rich phase grains are refined Sn-58Bi solder [243]. The addition of Ag nanoparticles can remark-
and dispersed in the matrix. For Sn-40Bi solder bearing P element ably refine the microstructure of solder. The degree of refinement
[237], when 0.1% P was added, the microstructure of alloy became changed with the size of Ag nanoparticles (31 nm, 76 nm,
finer, showing that the eutectic size was smaller and the b-Sn den- 133 nm), and the related interphase spaces are 1.57 mm, 1.16 mm
drites became more uniform. The solidification process has also and 1.34 mm, respectively. The greatest reduction of the interphase
undergone the transformation of b-Sn and Sn-Bi eutectic phase. spacing can be obtained with 1.0 wt% 76 nm Ag nanoparticles. Sn-
But there should also be some Sn-P compounds because the solu- 58Bi solder doped with Mo nanoparticles was investigated by Yang
bility of P in Sn is almost negligible and usually exists in the form of [244]. Sn-rich phase and Bi phase can be observed in the Sn-Bi sol-
SnP3IMCs. The addition of Sb can refine the microstructure of Sn- der with networks structure. The addition of Mo nanoparticles can
58Bi alloy [238]. The author used two aspects to explain the influ- refine the microstructures, and reduce the size of the phase space.
ence, one is the increase of nucleation sites with the addition of Sb, Moreover, the homogeneous microstructure of solders with the
and another is the reaction between Sb and Sn to form SbSn IMC. addition of Mo nanoparticles can be found. After adding for 10 days
The microstructures of Sn-58Bi-xIn (x = 1.0, 2.0, 3.0, 4.0, and and 20 days, the coarsened microstructures increase significantly
5.0 wt%) solder were investigated by Chen [239]. 1.0 wt% In can with increasing aging time. Due to the addition of Mo nanoparti-
Fig. 33. Sn-Bi phase diagram [230].
29
cles, the Sn-rich phase and Bi phase keep homogeneous in the sol- ous Cu in Sn-Bi solder can refine the whole structure. 1.0 wt% ZnO
ders. The influence of Ti nanoparticles on the microstructure of Sn- nanoparticles can be added into Sn-57.6Bi-0.4Ag solder to enhance
58Bi solder was investigated by Jiang [127]. With the addition of Ti the microstructure [248]. The microstructure of the matrix in Sn-
nanoparticles, the microstructures of Sn-Bi solder were refined Bi-Ag-ZnO solder shows a well refined microstructure. ZnO
remarkably, as shown in Fig. 34. Ti nanoparticles can play as the nanoparticles inhibit the growth of phases. The similar phenomena
nucleation site during the solidification processing. Eq. (27) can can be found for Sn-Bi solder with addition of ZrO2 nanoparticles
describe the relationship between the number of crystal nucleus, [249]. The Bi-rich phase can be refined remarkably. However, in
the nucleation rate and the rate of crystal growth. It is demon- Sn-58Bi solder doping 0.5 wt% Al2O3 nanoparticles, the microstruc-
strated that the addition of Ti nanoparticles can increase the nucle- ture shows no obvious variation compared plain Sn-58Bi solder
ation rate to refine the microstructure. The optimal content of Ti [130]. BaTiO3 nanoparticles can reduce the number and size of b-
nanoparticles is 0.1 wt%. However, with the further increase of Ti Sn phase significantly. The average b-Sn dendrite arm spacing of
nanoparticles content, due to the nanoparticles aggregation, the Sn-58Bi is 5.56 lm. For Sn-58Bi-xBaTiO3 (x = 0.5, 1, 2, 3) the values
coarsening microstructure can be found, which will weak the prop- are 2.58 lm, 1.88 lm, 2.34 lm, and 4.86 lm [250], which demon-
erties of solders. After the addition of 0.5 wt% W nanoparticles, it is strates the addition of BaTiO3 nanoparticles can enhance the
clear that the microstructure of Sn-57.6Bi-0.4Ag solder is refined refinement of the microstructure. SiC nanoparticles can also refine
considerably [245]. Moreover, the W nanoparticles will not react the microstructure of Sn-58Bi solder [251]. Due to the increase of
with Sn, Bi or Ag. Cu nanoparticles as additive can also refine the heterogenous nucleation sites and impeded phase or grain bound-
microstructure of Sn-58Bi solder [246]. The Cu nanoparticles can ary movement by SiC nanoparticles, the average size of eutectic
react with Sn to form Cu6Sn5 particles to provide the nucleation microstructure decreases up to 48.4%. With the addition of
sites for the Sn phase and Bi phase during soldering. However, 0.03 wt% GNSs [252], the average grain size can be changed from
when the content of Cu nanoparticles is 2.0–3.0 wt%, the refine- 1.63 lm to 0.75 lm with 54% reduction. Moreover, during
ment effect via inoculation is limited. 100 °C aging with 360 h, the microstructures of Sn-Bi and Sn-Bi-
GNSs solders are coarsened, and GNSs still refine the microstruc-
PðtÞ ¼ kðN=tÞ4=3 ð27Þ ture and reach the best in Sn-Bi with 0.03 wt% GNSs. Cu6Sn5
where PðtÞ is the number of crystal nucleus; kis a constant; N is the nanoparticles were synthesized and applied to improve Sn-58Bi
nucleation rate; t is the rate of crystal growth. solder [253]. The addition of Cu6Sn5nanoparticles can refine the
Porous Cu sheets with the pores per inch of 110 and 500 were microstructure, and the interphase spacing can be reduced obvi-
utilized to improve the microstructure of Sn-58Bi solder [247]. It ously. The optimal content of Cu6Sn5 nanoparticles is 0.05 wt%.
is clear that the microstructure of Sn-Bi-Cu solder consists of Bi- 1.2 wt% Al8B4O33 whisker can also refine the Bi-rich phase. The
rich phase, Sn-rich phase and porous Cu, and the Cu6Sn5 layer is grains can vary from bulk to fine dendrite morphology, and the
formed between the porous Cu and Sn-Bi solder, as shown in eutectic lamellar spacing decrease obviously [254]. For the addi-
Fig. 35. In the region surround by the porous Cu, the Bi-rich and tion of CNTs into Sn-58Bi solder, with the addition of 125 mg/L
b-Sn can be refined. The densely and uniformly distribution of por- CNTs. Sn-rich and Bi-rich phase can decreased obviously with
Fig. 34. Microstructures of Sn-Bi based solders: (a) Sn-Bi; (b) Sn-Bi-0.05Ti; (c) Sn-Bi-0.1Ti; (d) Sn-Bi-0.2Ti and (e) Sn-Bi-0.3Ti [127].
30
Fig. 35. Elemental maps of Sn-Bi-Cu solder [247].
25% and 18% reduction, respectively [255]. MWCNTs can also be W ad ¼ cgl ð1 þ cos hÞ ð30Þ
incorporated with Sn-Bi solder. The NWCNTS clusters can act as
where cgs is the gas/solid surface tension; cls is the liquid/solid sur-
the nucleation sites of Sn-Bi alloy to refine the microstructure
[256]. face tension; cgs is the gas/liquid surface tension; W ad is theadhe-
sion work; h is the contact angle.
3. Wettability
3.2. Spreading ratio and spreading area of solders
Wettability is an important index for lead-free solders, repre-
senting the ability of molten solder to infiltrate and adhere to the The spreading ratio can be utilized to evaluate the wettability of
metal substrate [257]. The wettability of molten solder on a metal lead-free solders [265]. According to Japanese Industrial Standard
substrate, which provides successful soldering and interconnec- JIS-Z3198-3 [239], the calculation equation of spreading ratio
tion, is very important for the formation of solder joint to deter- was shown as Eq. (31). The higher the spreading ration, the better
mine the reliability in service [258]. Three main methods can be the wettability of the lead-free solder is [266]. Moreover, the
utilized to evaluate the wettability of lead-free solders. Moreover, spreading area of solder can be calculated to determine the wetta-
Table 2 summarizes the wettability parameters of lead-free bility of solder according to Chinese National Standard GB/T1136-
solders. 2008 [267]. The sample can be photographed, input into the com-
puter, and the spreading are of lead-free solder can be calculated
3.1. Contact angle of lead-free solders by software. The parameters of wettability for calculation as shown
in Fig. 37. The larger the spreading area, the better the wettability
In order to describe the wettability, the Young-Dupre equations of the solder, which has been utilized to analyze the effect of TiO2
[259,260] were utilized as shown in Eq. (28)-Eq. (30). The relation- nanoparticles on the wettability of Sn-Ag-Cu solder [268]. It is
ship among contact angle, metal surface energy and adhesion found that the 0.1 wt% nanoparticles can improve the wettability
work. Fig. 36 shows the schematic illustration of molten solder of solder.
wettability on metal substrate. The contact angle [261,262] can Dh
be measured by experimental to analyze the wettability of lead- SR ¼ 100 ð31Þ
D
free solders. Therefore, the values of the contact angle as an impor-
tant index to analyze the wettability of solders [263,264]: Where SR is the spreading ration; D is the diameter of sample; h is
the maximum height of the spread solder after soldering.
0 < h < 30 indicating very good wetting, 30 < h < 40 express-

ing good wetting, 40 < h < 55 indicating acceptable wetting,
3.3. Wetting balance testing of lead-free solders
55 < h < 70 expressing poor wetting, and > 70 indicateing very
poor wetting. The parameter can be used to evaluate the wettabil- According to IPC/EIA J-STD-003B 2004 specification, the wetting
ity of lead-free solder. balance testing can be selected to determine the dynamic process-
cgs ¼ cgl cos h þ cls ð28Þ ing of wetting by measuring the wetting time and wetting force
[192]. As shown in Fig. 38, the wetting force between the immers-
W ad ¼ cgs þ cgl cls ð29Þ ing samples and molten solder can be quantitative calculated.
Short wetting force can determine the good wettability of lead-
31
Table 2
Wettability parameters of series of lead-free solders
Composition Additives Content Contact Wetting Spreading Spreading Surface Temperature Reference
(wt.%) angle force area ratio Tension
Sn3.0Ag0.5Cu Ga 0.5–1.5 260 °C 5 min [42]
2.0–10.0
Sn0.5Ag0.7Cu Ga 0.05–1.0 245–275 °C dipping [272]
Sn0.3Ag0.7Cu Mn nano 0.05 250 °C [152]
Sn3.8Ag0.7Cu Al nano 0.05–0.4 245 °C reflow [156]
Sn3.0Ag0.5Cu TiO2, GNS 0.015–0.3 250 °C, 30s [158]
Sn3.0Ag0.5Cu La2O3 nano 0.05 300 °C bath [163]
Sn3.0Ag0.5Cu AlN nano 0.03–0.6 250 °C bath [164]
Sn3.0Ag0.5Cu TiC nano 0.05,0.1,0.2 245 °C reflow [166]
Sn1.0Ag0.5Cu Fe2O3 nano 0.5 260 °C dipping [167]
Sn3.0Ag0.5Cu KGC micro 0.5–2.0 250 °C reflow [273]
Sn3.0Ag0.5Cu Fe2NiO4nano 0.5–2.5 250 °C,45s [274]
Diamond
nano
NiO nano
Fe2O3 nano
ITO nano
Sn0.3Ag0.7Cu Al2O3 nano 0.01–0.5 250 °C reflow [275]
Sn3.8Ag0.7Cu TiO2 nano 0.05–0.4 245 °C reflow [268]
Sn0.5Ag0.7Cu0.5Ga Pr 0.06–0.5 240–260 °C dipping [271]
Sn3.5Ag Cu-CNF 0.01–0.1 300 °C hotplate [183]
Sn0.7Cu0.05Ni Eu 0.024–0.105 240–260 °C dipping [192]
Sn0.7Cu Ni 0.05, 0.1 270–300 °C [195]
Sn0.7Cu S 0.02–0.08 260 °C dipping [197]
Sn0.7Cu0.2Ni In 0.1–0.3 270 °C 5 min [198]
Sn0.7Cu Ni Micro 0.025–0.04 250 °C reflow [201]
Sn0.7Cu GNSs 0.025–0.1 250 °C,20 min [202]
Sn0.5Cu3Bi Ag 0.25–1.0 No description [276]
Sn0.7Cu0.1Ni In 0.5–2 260 °C 10 min [277]
Sn9Zn Pr 0.01–0.25 235 °C dipping [209]
Sn9Zn Er 0.02–0.5 226 °C reflow [210]
Sn9Zn La 0.02–0.5 226 °C reflow [211]
Sn9Zn Y 0.02–0.3 226 °C reflow [212]
Sn9Zn Nd 0.015–0.5 235 °C,10s [213]
Sn9Zn In 0.5–2.0 200 °C,220 °C,240 °C, [216]
dipping
Sn9Zn Na 0.1–5.0 250 °C, 60–3600 s [221]
Sn8.55Zn0.5Ag Ga 1.0–3.0 230 °C,15s [223]
Sn58Bi Ti nano 0.05–0.3 175 °C reflow [127]
Sn58Bi Y 0.1–0.5 180 °C reflow [234]
Sn58Bi Ce 0.1–0.5 180 °C reflow [235]
Sn58Bi In 0.5–5.0 170 °C, 1790 °C, 1 min [239]
Sn58Bi BiTiO3 0.5–3.0 190 °C,5 min [250]
Sn20Bi GNS 0.02–0.1 250 °C,20 min [266]
Sn58Bi CuZnAl 0.05–0.4 175 °C reflow [242]
micro
Fig. 37. Parameters of wettability for calculation.
Fig. 36. Schematic illustration of molten solder wettability on metal substrate. maximum wetting force can be measured when the measured
force remains constant [270].
free solders. SAT5100 solderability test is frequently used to deter-

mine the wetting force and wetting time of lead-free solders [269]. 3.4. Effects of alloying elements and particles on the wettability of
When the metallic substrate is dipped into the molten lead-free lead-free solders
solder, the wetting fore can be obtained in the software, the dip-
ping speed, the immersion depth and the dwell time are the three Table 2 shows the data about the effects of alloying elements
important parameters for the experiments. During the testing, the and particles on the wettability of lead-free solders. Rare earth
32
found that the different value of Ga content can be obtained. The

discrepancy among the Ga content and the Ga effect are due to dif-
ferent development method of solders, reflowing temperature and
analytical method used. The wettability of Sn-0.7Cu-0.Ni solder
can be enhanced with the addition of In. The spreading can be
increased with the increase of In content [198], and parabola trend
can be demonstrated in the curve. The authors consider that the
decrease of melting temperature with the addition of In may be
the reason of enhancement of wettability. The similar effect of In
can be found in Sn-9Zn [216] and Sn-58Bi [239] solder.
For the metal nanoparticles (Mn, Al, Ti) or microparticles (Ni,
CuZnAl) as additives into lead-free solders, the wettability of sol-
ders can be improved significantly. For the metal particles, the par-
ticles and the solder matrix have good wettability. The particles are
Fig. 38. Wetting curve of lead-free solder [192]. easy to concentrate on the surface of molten solder, which can
easily reduce the surface tension of solder, and increase the fluid-
(RE) elements (Eu, Pr, Er, La, Y, Nd and Ce) as additives can improve ity, thus improve the wettability of the lead-free solders. For the
the wettability of lead-free solders, but the content of RE should be oxide particles (TiO2, La2O3, Fe2O3, Al2O3, TiO2 and BiTiO3) and
controlled with a small amount. The optimal range of RE is 0.03– other particles (AlN, TiC, KGC and GNS) as additives, the wettability
0.06 wt%. The valley bottom and valley peak can be observed in of lead-free solders can be enhanced in the literatures, as shown in
the wettability testing for wetting force, wetting time, contact Table 2. The addition of high surface energy nanoparticles can
angle, spreading area, spreading ratio and surface tension, respec- cause a decrease in surface energy between solder bearing
tively. Fig. 39 shows the wetting time and wetting force of Sn- nanoparticles and substrate to improve the wettability [158]. The
0.5Ag-0.7Cu-0.5 Ga-xPr solders with different temperatures optimal content of the nanoparticles can be found. For example,
[271]. Based on the evaluation of valley bottom and valley peak, the optimal addition of dual ceramic nanoparticles is 0.2 wt%.
the optimal content of Pr is 0.06 wt% for Sn-Ag-Cu-Ga solder with Moreover, the opposite results can also be found in the literature.
optimum wettability. Due to the active of rare earths, the RE can Chellvarajoo [274] attempted to add nanoparticles (Fe2NiO4, Dia-
segregate at the molten solder interface to decrease the interface mond, NiO, Fe2O3 and ITO) into Sn-3.0Ag-0.5Cu solder. The discrep-
tension, which can induce the enhancement of wettability of ancy among the different literatures are due to different
lead-free solders. However, when the content of RE as additive is development method of solders, reflowing temperature and ana-
more than optimal content, the reaction between RE and Sn to lytical method used. In addition, the uniform distribution of
form RE-Sn phase can be occurred. The RE-Sn phase can be easily nanoparticles in the solder is the main factor for the wettability
oxidized to form oxidation slags, which will hinder the wetting enhancement. If the nanoparticles are not evenly distributed in
of solders, so the wettability of lead-free solders can be reduced the solder, these nanoparticles will agglomerate on directly reduce
remarkably. the wettability of the solders. In addition to the wettability of the
Ga and In materials with low melting points were also selected lead-free solder can be affected by the type of nanoparticles. The
as additives into lead-free solders in Chen’s work [42]. With the size of nanoparticles also has a significant effect on the wettability
addition of 0.05–1.5 wt% Ga, the wettability of Sn-3.0Ag-0.5Cu sol- of the solders. The different of Fe2O3 nanoparticles size (20 nm,
der can be reduced. However, when the content of Ga is greater 50 nm and 200 nm) on the wetting force and wetting time has
than 2.0 wt%, the wettability can be enhanced obviously. For the been studied by Zhao [167]. 20 nm Fe2O3 nanoparticles can
Sn-Ag-Cu-7.0 Ga and Sn-Ag-Cu-10 Ga solders, the wettability of improve effectively the wettability of the Sn-Ag-Cu solder. the
solders is higher greatly than that of original Sn-Ag-Cu solder. 200 nm Fe2O3 nanoparticles show no obvious effect on the wetta-
But in Luo’s work [272], the addition of Ga (0.05–1.0 wt%) into bility. The results demonstrate that adding smaller-size Fe2O3
Sn-0.5Ag-0.7Cu solder can improve the wettability of solder signif- nanoparticles could enhance the wettability of composite solder
icantly with 0.5 wt% optimal content, as shown in Fig. 40. It is better than the larger-size Fe2O3 nanoparticles.
Fig. 39. Wettability of Sn-Ag-Cu-Ga-xPr solder: (a) Wetting time and (b) Wetting force [271].
33
Fig. 40. Wetting properties of Sn-0.5Ag-0.7Cu-xGa solder: (a) Wetting force and (b) Wetting time [272].
4. Melting behavior Adding 0.1 wt% of Fe, Co, Te and 2 wt% Bi into Sn-3.0Ag-0.7Cu
can alter the melting behavior of solder as shown in Fig. 41
The melting temperature of the lead-free solders is an impor- [142]. The melting of melting is changed from 218.9 °C to 221.1
tant index to evaluate the performance of lead-free alloys [278]. °C. The melting range between Tonest and Tend is slightly altered
The melting temperature of the solder directly determines the sol- by 1 °C and the value lies in the range of 5.0–6.0 °C, which is smal-
dering process parameters and the microstructure of the solder ler and can be suitable to the manufacture processing. The heat of
joint after soldering, and even affects the reliability of the lead- fusion DH as Eq. (32) can be calculated to be 190.5 and 102.7 J/g for
free solder joint in later service. Therefore, the investigation of Sn-3.0Ag-0.7Cu solder and Sn-3.0Ag-0.7Cu-TeFeCoBi solders. It is
melting behavior of lead-free solders bearing elements has been shown that the the addition of Fe, Te, Co and Bi can reduce the
focused, and a series of studies were published in journals and fusion heat of Sn-Ag-Cu for saving energy. Meanwhile, it is worth
conferences. noting that the degree of undercooling can be changed from 3.4
Table 3 shows the melting behavior of lead-free solders. Due to to 22.3 °C.
the low-temperature behavior of Ga and In, the addition of Ga or In
into lead-free solders, the low temperature of the composite solder DH ¼ KA=m ð32Þ
can be reduced easily. For Ga, with melting point around 30 °C, the
where A is the endothermic peak; m is the mass of the sample; K is
addition of Ga into Sn-3.0Ag-0.5Cu solder can decrease the melting
a calibration coefficient that depends on crucible shape.
temperature of the solder. Both the solidus temperature and liq-
1.0–4.0 wt% FeCo magnetic nanoparticles can also influence the
uids temperature can be reduced from 217.8 °C to 213.7 °C and
melting behavior of Sn-3.0Ag-0.5Cu solder [154]. Fig. 42 shows the
from 229.6 °C to 225.1 °C, respectively [42]. In Chen’s work
DSC profiles of the reflowed sample with different FeCo magnetic
[239], 0.5–5.0 wt% In were selected as additives into Sn-58Bi sol-
nanoparticles. During cooling the onest temperature varied from
der. The addition of In can decrease the solidus temperature and
197 °C to about 217 °C with the addition of 1.0 wt% FeCo. Under-
liquid temperature remarkably. It is found that 5.0 wt% In addition
cooling (temperature gap) between the onset temperature upon
lead to 19.8 °C decrease of the onset point corresponding to the
heating and cooling can be analyzed in this part. The FeCo exis-
solidus temperature, and 9.4 °C reduction of the offset point corre-
tance in the Sn-Ag-Cu solder can eliminates the large undercooling,
sponding to the liquid temperature.
shifting the solidification process from non-equilibrium to equilib-
For the Ni (0.15.0 wt%) as additive into Sn-3.5Ag solder, the
rium. With the addition of Zn into Sn-1.0Ag-0.3Cu solder [146], the
melting temperature of Sn-Ag solder can be increased with the
melting range of Sn-Ag-Cu-xZn is 13.8 °C, 6.6 °C (x = 2.0) and 7.5 °C
range (4.34–5.97 °C), and the melting range can be increased from
(x = 3.0), respectively. The authors consider that the new (Cu, Ag)5-
0 to 24.89 °C [176]. With the addition of Cu nanoparticles or Cu
Zn8 precipitate could nucleat much more easily than b-Sn and
microparticles (0.7 wt% and 3.0 wt%), 3–4 °C reduction of melting
other IMC, which is the reason of the decrease of melting range.
points of Sn-3.5Ag solder can be found [177]. Moreover, the addi-
Moreover, the Zn addition can also decrease the under cooling
tion of 0.2 wt% Cr into Sn-0.7Cu alloy can enhance the melting tem-
from 4.2 to 2.5 °C.
perature by about 3 °C [194]. Other elements (Fe, Zn, Co, Mn, Sb,
Ag, Bi, Ce, Y, Cu, S, etc.) and nanoparticles/microparticles (TiO2,
GNS, NiO, SiC, Fe2O3, SrTiO3, Al2O3, ZrO2, KGC, Fe2NiO4, Diamond, 5. Mechanical properties
ITO, Si3N4, etc.) have little effect on the melting temperature. The
variation range may be 1–3 °C. For example, with the addition of Solder joints play the role of mechanical support and electrical
KGC into Sn-3.0Ag-0.5Cu solder, the average melting temperatures connection in electronic devices [283]. So the study of mechanical
of Sn-Ag-Cu-Xkgc (0, 0.5, 1.0, 1.5, 2.0) are 220.86 °C, 220.55 °C, properties of lead-free solder and solder joints has become an
220.56 °C, 221.01 °C, 221.11 °C [273], respectively. Little effect of important index to evaluate the properties. The research on
KGC can be demonstrated. These data suggest that there is no need mechanical properties is mainly aimed at tensile and shear testing,
to change the reflow soldering processing while adopting these hardness, and creep experiments. For the series of lead-free solders
novel lead-free solders. The melting range and undercooling are bearing alloying elements or particles, the influence effect of alloy-
the critical parameters for lead-free solders to determine phase ing elements or particles on mechanical properties can be attribu-
precipitations and the properties. The narrow melting range of sol- ted to particle strengthening and solid solution strengthing [284].
ders is beneficial in avoiding vibrational defects like fillet lifting, Table 4 shows the mechanical parameters of lead-free solders
porosity, and hot tearing during wave soldering [279]. and solder joints investigated by different researchers.
34
Table 3
Melting behaviors of lead-free solders
Composition Additives Content (wt.%) Melting of melting Undercooling Melting range Reference
Sn-3.0Ag0.7Cu Fe, Te, Co and Bi 0.1, 2.0 [142]
Sn3.0Ag0.5Cu Ga 0.5–1.5 [42]
Sn1.0Ag0.5Cu Fe 0.1–0.5 [144]
Sn1.0Ag0.3Cu Zn 2.0, 3.0 [146]
Sn1.0Ag0.5Cu Zn 1.0 [147]
Sn3.0Ag0.5Cu
Sn3.0Ag0.5Cu Sb 0.2 [148]
Sn3.0Ag0.5Cu Mn 0.2 [148]
Sn3.0Ag0.5Cu Zn 0.2 [148]
Sn3.0Ag0.5Cu Co nano 0.2,0.5,0.8 [153]
Sn3.0Ag0.5Cu FeCo nano 1.0–4.0 [154]
Sn3.0Ag0.5Cu TiO2, GNS 0.015–0.3 [158]
Sn3.0Ag0.5Cu NiO nano 0.5, 1.5, 2.5 0.5NiO [58]
=1.5NiO
2.5NiO
Sn1.0Ag0.5Cu SiC nano 0.35, 0.75 [165]
Sn3.0Ag0.5Cu TiC nano 0.05,0.1,0.2 [166]
Sn1.0Ag0.5Cu Fe2O3 nano 0.5 [167]
Sn3.0Ag0.5Cu SrTiO3 nano 0.5 [168]
Sn0.3Ag0.7Cu Al2O3 nano 0.01–0.5 [275]
Sn1.7Ag0.7Cu Te 0.2 [280]
Sn1.7Ag0.7Cu Co 0.5 = [280]
Sn3.0Ag0.5Cu ZrO2nano 0.5–3.0 [161]
Sn3.0Ag0.5Cu KGC micro 0.5–2.0 [273]
Sn3.0Ag0.5Cu Fe2NiO4nano 0.5–2.5 [274]
Diamond nano
NiO nano
Fe2O3 nano
ITO nano
Sn3.0Ag0.5Cu Sn nano 1.0–5.0 [281]
Sn3.5Ag Bi 0.3 [172]
Sn1.0Ag Ti 0.2, 0.6 [174]
Sn3.5Ag Ti, Cd 0.27 [175]
Sn3.5Ag Ni 0.1–5.0 [176]
Sn3.5Ag Cu nano/micro 0.7, 3.0 [177]
Sn3.5Ag Ge 0.1,0.3 [282]
Sn0.7Cu(Ag) Ce 0.005–0.171 [189]
Sn0.7Cu0.05Ni Eu 0.024–0.105 [192]
Sn0.5Cu Al 0.01–0.05 No effect [193]
Sn0.7Cu Cr 0.2 [194]
Sn0.7Cu Ag, In 2.0 In In [196]
Ag Ag
Sn0.7Cu S 0.02–0.08 [197]
Sn0.7Cu0.2Ni In 0.1–0.3 [198]
Sn0.7Cu Bi 0.7,1.3 [199]
Sn0.7Cu GNSs 0.025–0.1 [202]
Sn0.7Cu Si3N4 micro 0.5–1.5 [203]
Sn0.7Cu ZnO nano 0.1–1.0 [205]
Sn0.5Cu3Bi Ag 0.25–1.0 [276]
Sn0.7Cu0.1Ni In 0.5–2.0 [277]
Sn0.7Cu Ni 0.5–2.0 0.5,1.0 [267]
1.5,2.0
Sn6.5Zn Ni, Sb 0.5 Ni =Ni [214]
Sb Sb
Sn9Zn Ag micro 0.5–1.5 [224]
Sn9Zn Sb nano 0.5–1.5 [225]
Sn9Zn Al2O3 nano 3.0 [226]
Sn9Zn CeO2 nano 0.3–0.9 [228]
Sn58Bi Ti nano 0.05–0.3 [127]
Sn58Bi Ag 1.0 [233]
Sn58Bi Y 0.1–0.5 [234]
Sn58Bi Ce 0.1–0.5 [235]
Sn58Bi Ti 0.5,1.0 [240]
Sn58Bi Cu nano 3.0 [246]
Sn58Bi In 1.0–5.0 [239]
Sn40Bi Cu, Zn 0.1, 2.0 [241]
Sn58Bi CuZnAl micro 0.05–0.4 [242]
35
Fig. 41. DSC results during heating (endothermal): (a) Sn-3.0Ag-0.7Cu solder and (b) Sn-3.0Ag-0.7Cu-TeFeCoBi solder [142].
similar promotion effect in Sn-3.5Ag [172], Sn-0.7Cu [199] and

Sn-58Bi [215] solders. Te and Co elements can also enhance the
mechanical properties of Sn-Ag-Cu solders. For Sn-1.7Ag-0.7Cu-
0.7Te and Sn-1.7Ag-0.7Cu-0.7Co solders, the stress levels and duc-
tility are significantly higher at all testing temperatures [280] with
higher resistance to necking. The addition of Ag, Sb, Cu, Zn, Na, Ti,
Ni elements can react with the matrix elements (Sn or Cu) of lead-
free solders to form particles and refine the microstructure, which
can strengthen the mechanical properties of lead-free solders or
solder joints. Cr elements can also improve mechanical properties.
CrSn2 particles in Sn-0.7Cu-0.2Cr solder [194] and ZnCr particles in
Sn-8Zn-3Bi-0.3Cr solder [220] can be observed, and no particles
containing Cr in Sn-3.5Ag-xCr (x = 0, 1, 3, 5 wt%) can be found
[173]. So for the effect mechanism of Cr element should be studied
systematically. For the Al element, the refining effect and Al parti-
cles strengthening are suggested as the enhancement mechanism
of Sn-30Bi solder joints [236].
For Sn-1.0Ag-0.5Cu-xFe (x = 0.1,0.3,0.5) solders [144], the addi-
Fig. 42. DSC profile of Sn-Ag-Cu-xFeCo [154].
tion of Fe can lead to the formation of bulk FeSn2 IMC. The particle
diameters are even more than 10 lm. These bulk particles can
decrease the mechanical properties, which indicates that the
5.1. Shear and tensile properties of lead-free solder joints mechanical properties of solder joints are related to particles size.
For this problem, Chen [167] investigated the effect of different
For lead-free solders bearing alloying elements, based on shear Fe2O3 sizes on the shear strength of Sn-1.0Ag-0.5Cu solder. The
testing and tensile testing, the shear strength and tensile strength shear strength of solder with 20 nm particles addition is
can be enhanced effectively except for Sn-1.0Ag-0.5Cu-xFe, Sn- 45.1 MPa and increased by 33% compared to the original Sn-Ag-
40Bi-xP, Sn-58Bi-xIn. The data can be obtained from Table 4. For Cu solder. But with the addition of 20 nm particles, the shear
a small amount addition of rare earth (Ce, Yb, Eu, etc.) into lead- strength of solder can be decreased remarkably. So for the investi-
free solders, the RE can react with Sn matrix to form small RESn3 gation of lead-free solders, the small size particles are the selection
particles. The precipitated particles can strengthen the solder or to enhance the mechanical properties.
solder joints. For Sn-3.8Ag-0.7Cu solder joints with optimal Yb con- The addition of P into Sn-40Bi solder can reduce the tensile
tent (0.05 wt%), the tensile force of Sn-Ag-Cu solder joints in QFP strength [237] in Wang’s work. The P as additives can induce the
devices gives a 25.4% increase after soldering [36]. For Sn-3.5Ag- formation of voids in the solder matrix, and the voids can provide
0.7Cu and Sn-3.5Ag-0.7Cu-1.5 Ga solders [40], the shear strength the opportunity for the crack during loading. The mechanical prop-
of Sn-Ag-Cu/Cu and Sn-Ag-Cu-Ga/Cu solder joints are 29 MPa erties can be decreased obviously. Chen [239] added In into Sn-
and 33 MPa, respectively, as shown in Fig. 43, which demonstrates 58Bi solder. The results show that the tensile strength of Sn-Bi sol-
that the addition of 1.5 wt% Ga can enhance the shear strength of der with In addition decreases slightly, and the maximum elonga-
Sn-Ag-Cu/Cu solder joints. tion reaches 44.5% increasing 122.5% in Sn-Bi-2.5In solder
For the addition of 0.05 wt% Fe and 1 wt% or 2 wt% Bi, the ulti- compared with original Sn-Bi solder, as shown in Fig. 44. For Sn-
mate tensile stress of Sn-1.0Ag-0.25Cu solder can be increased 58Bi solder bearing Cu6Sn5 particles, the Cu6Sn5 particles can also
from 27.5 MPa to 56 MPa, and increased yield strength from decrease the tensile strength of Sn-Bi solder [253]. The authors
21 MPa to 41.8 MPa. Moreover, after aging (125 °C for 30 days), proposed that the phenomenon can be attributed to the weak
the Sn-Ag-Cu-Fe-Bi solder has stabilized mechanical properties, bonding between the Sn-Bi matrix and the Cu6Sn5 particles. 0.1–
which can be attributed to the prevention of Cu and Sn interaction, 1.0 wt% CoPd nanoparticles as additives can also decrease the shear
and the decrease of IMCs coarsening rate [145]. Bi element has strength of Sn-3.0Ag-0.5Cu solder joints [285]. The variation trend
36
Table 4
Mechanical properties of lead-free solders and solder joints
Composition Additives Content (wt.%) Shear force Tensile force Hardness Creep resistance Reference
Sn3.8Ag0.7Cu Yb 0.025–0.5 25.4% [36]
Sn3.8Ag0.7Cu Eu 0.02–0.5 [296]
Sn3.8Ag0.7Cu Ce 0.03 [297]
Sn3.5Ag0.7Cu Ga 1.5 [40]
Sn0.5Ag0.7Cu Ga 0.05–1.0 [272]
Sn3.0Ag0.7Cu Fe, Te, Co and Bi 0.1,2.0 [142]
Sn1.0Ag0.5Cu Fe 0.1–0.5 [144]
Sn1.0Ag0.5Cu Fe, Bi 0.05, 1.0,2.0 103.6% [145]
Sn1.0Ag0.3Cu Zn 2.0, 3.0 [146]
Sn0.7Ag0.5Cu Bi and Ni 3.5, 0.05 124.5% [149]
Sn0.7Ag0.5Cu Bi and Ni 3.5, 0.05 [292]
Sn3.8Ag0.7Cu CuZnAl 0.5 [68]
Sn3.0Ag0.5Cu NiO nano 0.5, 1.5, 2.5 50% [58]
Sn3.0Ag0.5Cu Ni nano 0.5 11.2% 16.7% [150]
Sn0.3Ag0.7Cu Mn nano 0.02–0.3 24.8% [152]
Sn3.8Ag0.7Cu Al nano 0.1–0.4 [156]
Sn3.0Ag0.5Cu SnO2 nano 0.1–1.0 66.7% [160]
Sn3.5Ag0.5Cu ZnO nano 0.5 [162]
Sn3.0Ag0.5Cu La2O3 nano 0.01–0.1 [163]
Sn3.0Ag0.5Cu AlN nano 0.03–0.6 [164]
Sn3.0Ag0.5Cu TiC nano 0.05,0.1,0.2 [166]
Sn1.0Ag0.5Cu Fe2O3 nano 0.5 20 nm [167]
50 nm
200 nm
Sn3.0Ag0.5Cu SrTiO3 nano 0.5 [168]
Sn3.0Ag0.5Cu KGC micro 0.5–2.0 [273]
Sn3.0Ag0.5Cu Fe2NiO4nano 0.5–2.5 [274]
Diamond nano
NiO nano
Fe2O3 nano
ITO nano
Sn0.3Ag0.7Cu Al2O3 nano 0.01–0.5 [275]

Sn1.7Ag0.7Cu Te 0.2 [280]
Sn1.7Ag0.7Cu Co 0.5 [280]
Sn3.8Ag0.7Cu TiO2 nano 0.05–0.4 [268]
Sn0.5Ag0.7Cu0.5Ga Pr 0.06–0.5 [271]
Sn3.8Ag0.7Cu CuZnAl 0.5 [67]
Sn0.3Ag0.7Cu GNSs 0.01–0.09 [298]
Sn3.0Ag0.5Cu Sb 25–31 [299]
Sn3.0Ag0.5Cu CoPd nano 0.1–1.0 [300]
Sn3.5Ag0.7Cu MW-CNT [294]
Sn3.0Ag0.5Cu Ag-GNSs 0.03–0.2 [295]
Sn3.5Ag Bi 0.3 [172]
Sn3.5Ag Cr 1,3,5 19% 22.37% [173]
Sn1.0Ag Ti 0.2, 0.6 [174]
Sn3.5Ag Ti, Cd 0.27 [175]
Sn3.5Ag Ni 0.1–5.0 (0.1,1,3,5) (0.3,0.7,1,3,5) [176]
(0.1,0.3,1,3,5)
Sn3.5Ag Cu nano/micro 0.7, 3.0 [177]
Sn3.5Ag Mo, Ni nano 0.5–1.5 79.62% [179]
81.48%
Sn3.5Ag Cu-CNF 0.05 [183]
Sn3.5Ag ZnO nano 0.3 [184]
Sn3.5Ag POSS nano 1.0–5.0 18.4% [186]
Sn0.7Cu Ce 0.697–0.784 [189]
Sn0.7Cu0.05Ni Eu 0.024–0.105 [192]
Sn0.7Cu Cr 0.2 [194]
Sn0.7Cu Ag, In 2.0 [196]
Sn0.7Cu0.2Ni In 0.1–0.3 [198]
Sn0.7Cu Bi 0.7, 1.3 [199]
Sn0.7Cu Ni Micro 0.025–0.04 [201]
Sn0.7Cu GNSs 0.025–0.1 [202]
Sn0.7Cu Si3N4 micro 0.5–1.5 [203]
Sn0.7Cu SiC nano 0.1–0.3 [204]
Sn0.7Cu ZnO nano 0.1–1.0 [205]
Sn0.7Cu TiO2 nano 1.0 [206]
Sn0.5Cu3Bi Ag 0.25–1.0 [276]
Sn0.7Cu0.1Ni In 0.5–2 [277]
(continued on next page)
37
Table 4 (continued)
Composition Additives Content (wt.%) Shear force Tensile force Hardness Creep resistance Reference
Sn0.7Cu Ni 0.5–2.0 [267]
Sn0.7Cu0.05Ni CNT, GNS 0.5, 0.05 [301]
Sn0.7Cu Ag nano 1.0 (vol.%) [293]
Sn9Zn Pr 0.01–0.25 28.7% 38% [209]
Sn9Zn Er 0.02–0.5 [210]
Sn9Zn La 0.02–0.5 fx3 30% [211]
Sn9Zn Y 0.02–0.3 27.2% 24.1% [212]
Sn9Zn Nd 0.015–0.5 26.6% [213]
Sn6.5Zn Ni, Sb 0.5 fx3 [214]
Sn9Zn Bi 1.0–3.0 [215]
Sn9Zn Ag,Cu 15, 0.7 fx3 [217]
Sn9Zn0.5Al Sb 0.5–1.5 [219]
Sn8Zn3Bi Cr 0.1–0.5 [220]
Sn9Zn Na 0.1–5.0 [221]
Sn8.55Zn0.5Ag Ga 1.0–3.0 116% [223]
Sn9Zn Ag micro 0.5–1.5 [224]
Sn9Zn Sb nano 0.5–1.5 [225]
Sn9Zn Al2O3 nano 0.5–3.0 [226]
Sn9Zn CeO2 nano 0.3–0.9 [228]
Sn58Bi Ti nano 0.05–0.3 [127]
Sn58Bi Ag 1.0 [233]
Sn58Bi Y 0.1–0.5 71.09% 8.9% [234]
Sn58Bi Ce 0.1–0.5 8.87% [235]
Sn30Bi Al 0.3–1.0 [236]
Sn40Bi P 0.1 [237]
Sn58Bi Ti 0.5, 1.0 [240]
Sn57.6Bi0.4Ag W nano 0.5 [245]
Sn58Bi In 1.0–5.0 [239]
Sn40Bi Cu, Zn 0.1, 2.0 [241]
Sn58Bi Cu porous [247]
Sn57.6Bi0.4Ag ZnO nano 1.0 [248]
Sn58Bi ZrO2 nano 0.5 [249]
Sn58Bi BiTiO3 nano 0.5–3.0 [250]
Sn58Bi SiC nano 0.5 g/1 L [251]
Sn58Bi GNSs nano 0.03–1.0 [252]
Sn58Bi Cu6Sn5 nano 0.03–0.1 [253]
Sn30Bi Cu-MWCNTs 0.5–3.0 [302]
Fig. 43. Shear testing of Sn-Ag-Cu/Cu and Sn-Ag-Cu-Ga/Cu solder joints [40]. Fig. 44. Mechanical properties of Sn-Bi-In solder [239].
can not show any considerable enhancement of mechanical prop- The addition of metal particles (Ni, Al, Ag, Sb, Ti, W, CuZnAl, etc.)
erties of Sn-Ag-Cu/Cu solder joints. The authors analyze the degra- and non-metal particles (ZnO, La2O3, AlN, TiC, SrTiO3, KGC, Al2O3,
dation effect of CoPd nanoparticles using interfacial IMC TiO2, Cu-CNTs, ZnO, GNSs, Si3N4, SiC, ZnO, CeO2, ZrO2, BiTiO3,
microstructure. The CoPd nanoparticles can increase the IMC thick- etc.) into series of lead-free solders, the shear strength and tensile
ness of both Cu6Sn5 and Cu3Sn, which should be directly connected strength can be improved obviously. Two factors [184] can be used
with the decrease of shear strength. to explain the enhancement: a) pinning action of particles as addi-
38
tives which subsequently impede sliding of the grain boundaries as the effect mechanism of the tensile strength for a series of lead-
can be deduced, and b) the dispersive strengthening of the matrix free solders or solder joints as shown in Fig. 45. When the deforma-
by finely dispersed particles. In the solder joints, the relationship tion of solder happened, more and more dislocation began to be
between dislocation density q and strain e can be expressed as fol- produced. The dislocation density and is proportional to the strain
lows [286]: rate, so dislocation density increases with the increase of strain
rate. The result will lead to further increase the stress to increase
q / e; dq=dt / de=dt ¼ e_ ð33Þ the ultimate tensile strength of solders. In addition, the interaction
Eq. (33) shows that the dislocation density is proportional to the among dislocations results in the formation of the dislocation
strain rate. As the strain rate increases, the dislocation density delivery. This not only increases the length of the dislocation but
increases. Therefore, when the strain rate increases, the dislocation also the formation of the dislocation in this way the delivery parts
propagation rate increases due to the shortened movement time of than no formation of the dislocation delivery less mobile. There-
the dislocation. The dislocation theory can be utilized to explain fore, dislocation delivery can reduce the dislocation motion, which
Fig. 45. The mechanism for dislocation multiplication [286].
39
can enhance the tensile properties of the composite solder. In the

Sn-3.8Ag-0.7Cu solder, the Al nanoparticles can be found at the
grain boundaries in the solder matrix. The dislocation/particles
interactions phenomenon can be observed using TEM [6], further
demonstrating the enhancement of mechanical property of lead-
free solders or solder joints bearing nanoparticles. Moreover, Eid
[287] analyzed the strengthening mechanisms of ZnO nanoparti-
cles. Five effects can be used for the investigation including grain
refinement, formation of internal thermal stress due to different
CTE between the Sn matrix and ZnO particles, Orowan strengthen-
ing mechanism, effective load transfer between the Sn matrix and
ZnO particles, and hardening due to the strain misfit between in
gradients of solders bearing nanoparticles. Eq. (34)-Eq. (40) can
be used to calculate the increase in the yield strength of lead-
free solders bearing nanoparticles.
rCYS ¼ rm þ Dr ð34Þ Fig. 46. Microhardness of Sn-Ag-Cu and Sn-Ag-Cu-La solders before and after
thermal aging at 150 °C [288].
qffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
2
rCYS ¼ rm þ Drgs þ ðDrCTE Þ2 þ ðDrOrowan Þ2 ð35Þ
1=2
10.14 to 9.45. The authors suggest that the new indium-containing
Drgs =kd (36) phases formation in the matrix is the decrease reason of hardness.
pffiffiffiffi Moreover, the addition of Bi, Ni, Cu, Zn, Cr, Ti, and Ag can obvi-
DrCTE ¼ aGm b q ð37Þ
ously enhance the hardness of lead-free solders. Bi is a solid solu-
12 am ap T process T test V p tion in Sn and enrich in the solder matrix, which plays the role of
q¼ ð38Þ solid solution strengthening. Ni can refine the IMCs in the solder,
bd 1 V p
so the Bi and Ni can improve the hardness of Sn-0.7Ag-0.5Cu solder
[149]. For Sn-Bi solder, the hardness increases with the addition of
0:13Gm b d
DrOrowan ¼ ln ð39Þ Cu and Zn, the refinement of microstructure, and the fromation of
k 2b secondary particles in the matrix can be proposed to explain the
qffiffiffiffiffiffiffiffiffiffiffiffiffiffi phenomenon [241]. With the addition of Cr into Sn-3.5Ag solder,
k ¼ d 3 1=2V p 1 ð40Þ the hardness of solder shows an improvement by 22.37% compared
to the original Sn-Ag solder [173]. The Eq. (41) can be used to cal-
where rCYS is the yield stress of solder bearing nanoparticles; rm is culate the Vickers hardness of solder. The addition of Ti into Sn-Cu
the yield stress of original solder; Dr is the increase of yield stress; and Sn-Ag solders can effectively increase the hardness of solder
Drgs is the grain size strengthening; DrCTE is the dislocation [174]. The formation of Ti2Sn3 can stabilize the microstructure to
strengthening; DrOrowan is the dispersion strengthening;q is the dis- enhance the properties. The hardness of solders is so sensitive to
location density; k is the interparticle spacing;V p is thevolume frac- the microstructures of lead-free solders. The hardness of Sn-
tion of the nanoparticles; b is the Burgers vector od the matrix; d is 0.5Cu-3.0Bi solder is found to be increasing with the addition of
the particles size; Gm is the shear modulus of the matrix; k is a Ag [276].
constant.
1:854F
Hm ¼ ð41Þ
5.2. Hardness of lead-free solders L2
where F is the applied load (measured in kilograms-force); L2 is the
Hardness is defined that the local resistance of a material to the area of the indentation (measured in square millimeters).
pressure of a hard object into its surface. The higher the hardness, For the addition of metal particles (Ni, Mn, Cu, Mo, Ni, Ag, Sb,
the greater the mechanical strength, and the greater the hardness, etc.) and non-metal particles (NiO, SnO2, La2O3, AlN, TiC, Fe2NiO4,
the worse the ductility. So hardness is also an important index to Diamond, Fe2O3, ITO, Al2O3, CNTs, POSS, Si3N4, CeO2, GNSs, etc.),
evaluate the properties of lead-free solders. the hardness of lead-free solders can be enhanced obviously. With
Rare earth La as additives can decrease the hardness of Sn- the addition of Mo nanoparticles into Sn-58Bi solders, the hardness
3.0Ag-0.5Cu solder [288]. Fig. 46 shows the hardness value of both can be improved obviously. After aging, the hardness can be
solders with different aging times at 150 °C. The hardness of Sn-Ag- reduced with the increase of aging time for all specimens, but
Cu-0.4La consistently displays lower values than Sn-Ag-Cu solder the hardness of solders doped Mo nanoparticles shows higher than
due to the formation of bulk IMCs, which also demonstrate that that of Sn-Bi solder [244]. For the addition of POSS, the microhard-
excessive rare earth can degrade the properties of lead-free solders. ness of Sn-Ag-3POSS solder enhanced about 18.4% compared with
For Sn-58Bi solder, with the addition of rare earth Y, the hardness that of the Sn-3.5Ag solder [186]. Due to the addition of particles
can be enhanced obviously [234]. 8.9 wt% increments with 0.4 wt% into lead-free solders, the theory of dispersion strengthening can
Y addition can be found. In view of the above two literatures, the be used to explain the effect mechanism [289]. Eq. (42) can be used
additional amount of rare earth elements is given. But the actual to express the stress acting on the surface of particles using the
content is not given using testing after preparation, because after movement of dislocations.
the addition of rare earth elements, a certain amount of rare earth
elements will be lost during the transformation of solder into sol- s ¼ ns0 ð42Þ
der joints. So the actual content of rare earth should be tested, where s is the stress acting on the surface of particles; n is the num-
which is so important for the investigation. For the addition of In ber of dislocations; and s0 is the yield stress of the solder.
into Sn-Cu-Ni solder [198,277], the deteriorating effect of hardness
can be demonstrated. When the In content increases from 0.1 to pð1 mÞLs0
n¼ ð43Þ
0.3 wt%, the hardness of Sn-0.7Cu-0.2Ni-xIn solder decreases from Gb
40
where L is the average spacing between the secondary particles; b is particles can be observed to be the rate-controlling creep mecha-
the Burgers vector, m is the Poisson’s ratio, and G is the shear elastic nisms as shown in Fig. 48 [290]. So for novel lead-free solders bear-
modulus. ing alloying elements or particles, the evolution of the particle in
the matrix can influence the creep performance of solders or solder
pð1 mÞLs20
s¼ ð44Þ joints. The minimum creep rate is one of the most significant
Gb parameters of creep resistance in the assessments of lead-free
According to the above formulate, the yield stress of the solder solders.
can be calculated as follows. The tensile creep tests of Sn-1.0Ag-0.5Cu-0.02Ni solder have
sffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi been conducted by Chen [291]. A small amount of metal addition
Gbs into lead-free solder usually increases the creep resistance due to
s0 ¼ ð45Þ
pð1 mÞL the formation of IMC particles. The Ni addition can refine the
microstructure of Sn-Ag-Cu, and different types of creep constitu-
If s is defined as the fracture stress of the secondary particles tive models for Sn-1.0Ag-0.5Cu-0.02Ni can be obtained as Eq.
and m is a constant, so with the decrease of average spacing of (46)-Eq. (49). Kong [292] investigated the 3.5 wt% Bi and 0.05 wt
the secondary particles. the yield stress of the alloy increases. % Ni are coupled added into Sn-0.7Ag-0.5Cu solder. The indenta-
Hence, the finer and dispersed secondary particles can enhance tion creeping rate of the Cu/solder/Cu solder joints are declined
the mechanical properties of the alloy effectively. From the exper- 8.8157–16.059% at four different maximum loads. The creep stress
imental results, the average spacing L between Ag3Sn particles can exponent can be increased 32.175%, so the Bi and Ni can effectively
be obtained, so the L1 =L2 ¼ 1:69, and leading to s1 =s2 ¼ 1:30, based improve the creep resistance of the Cu/Sn-0.7Ag-0.5Cu/Cu solder
on experiments. Ht1 =Ht2 ¼ 1:18, the data is close to the above the- joints. In addition, for Sn-3.5Ag solder, the 0.3 wt% Ni can also
oretical prediction using dispersion strengthening theory, which decrease the creep rate of solder [176] to increase the creep resis-
further demonstrates the dispersion strengthening theory can be tance. For Sn-6.5Zn solder, Ni and Sb were added into the solder
used to explain the enhancement effect of POSS as an additive into [214]. (Ni, Zn)3Sn4 particles in solder with 0.5 wt% Ni and Sb solid
Sn-3.5Ag solder. solution effect in solder with 0.5 wt% Sb can increase the creep
resistance of solder.
5.3. Creep behavior of lead-free solders Nortons’s power-law model:

For series of lead-free solders, the melting temperature is very 6282:7
e_ c ¼ 2:39 107 r8:90 exp ð46Þ
low. For example, the melting temperature of eutectic Sn-Ag-Cu T
solder is 217 °C, absolute temperature is 490 K, for the room ambi- Double power-law model:
ent, the working temperature is more than 0.6 times the melting
temperature of solders. At such high homologous temperature, 4883:1
e_ c ¼ 9:87 107 r7 exp
the solder joints are subjected to remarkably creep deformation T

of series of lead-free solders. In addition, the actual service temper- 10 13 8949:2
ature of the solder joint is significantly higher than that of room þ 5:01 10 r exp ð47Þ
T
temperature. The creep deformation of the solder joint is more sev-
ere, so the creep behavior is an important index to study the solder Garofalo hyperbolic sine model:
and solder joint performance.
7024:2
Fig. 47 shows the typical creep deformation of a viscoplastic e_ c ¼ 3:94 104 ½sinhð0:0607rÞ 6:32 exp ð48Þ
T
material [290], which exhibits typical three stages characteristics.
The primary creep regime is defined by a region in which the strain Exponential model:

rate gradually decreases over time, and work hardening phe-
r 7744:3
nomenon can be found. For the secondary or steady-state creep e_ c ¼ 277:4exp exp ð49Þ
2:11 T
regime, the creep strain rate is stable and becomes constant. In
the tertiary creep regime, the strain rate increases over time, lead- where e_ c is the steady-state creep strain rate; r is the applied stress,
ing to creeping rupture. The three stages can be found in lead-free and T is the absolute temperature.
solders. The particles play an important role in the creep behavior The creep behavior of Sn-3.0Ag-0.7Cu and Sn-3.0Ag-0.7Cu-0.1
of solder. For example, in Sn-Ag solder, dislocation detachment Fe-0.1Te-0.1Co-2.0Bi solders were investigated by EI-Taher [142].
mechanism and Orowan climb mechanism form nanoscale Ag3Sn The creep parameters of solders are fitted for Garofalo hyperbolic
sine model as shown in Eq. (50). Based on testing and fitting, it is
found that the values of n and Q are increased with the addition
of Fe, Te, Co, and Bi in Sn-Ag-Cu solder. Due to the formation of
new (Cu, Co)6Sn5, SnTe IMCs particles and precipitated Bi particles,
the stress exponent in Sn-Ag-Cu-Fe-Te-Co-Bi is higher than that in
Sn-Ag-Cu solder, which demonstrates the reduction of creep rate.
Moreover, the dislocation climb controlled by pipe and lattice dif-
fusion are considered as the dominant deformation mechanisms.
For the Sn-1.0Ag-0.3Cu solder with the addition of Zn [146], the
creep rate can be reduced significantly. The creep fracture time
of Sn-Ag-Cu-3.0Zn is almost twice as high compared with original
Sn-Ag-Cu solder, indicating that Sn-Ag-Cu-3.0Zn solder has much
more creep resistance (360%) than that of plain Sn-Ag-Cu solder.
The addition of Zn can react to form (Cu, Ag)5Zn8 particles and
refine the Ag3Sn particles. Fine particles could act as a barrier for
dislocations to enhance the creep resistance. Moreover, the creep
Fig. 47. Typical creep curve for a viscoplastic material [290]. parameters of Sn-Ag-Cu, Sn-Ag-Cu-2.0Zn, and Sn-Ag-Cu-3.0Zn are
41
Fig. 48. Recovery of dislocations from Ag3Sn particles (a) Orwan climb mechanism; (b) dislocation detachment mechanism [290].
fitted for Garofalo hyperbolic sine model as shown in Eq. (51)-Eq. primary creep stage time can be decreased dramatically. The
(53). improvement can be attributed to the interactions between the
dislocations and nanoparticles, which can slow down the climb
e_ ¼ A½sinhðarÞ n expðQ =RT Þ ð50Þ of dislocations. Moreover, the addition of 0.5 wt% CuZnAl
microparticles can reduce the creep strain of Sn-3.8Ag-0.7Cu solder
where e_ is the steady-state creep strain rate; a is the tensile stress
joints in service can enhance the reliability of solder joints.
multiplier; r is steady flow stress; A is the materials related coeffi-
!
cients; n is the stress exponent; R is the gas constant; Q is the acti- G s 10:21 85:5 9:73 103 ðs=GÞ
vation energy. e_ ¼ 3:23 1032 exp
T G RT
!
45:0 115 1:02 104 ðs=GÞ
e_ ¼ 3:1 104 ½sinhð0:05760rÞ 5:1 exp ð51Þ
þ 6:93 1029
G s 7:7
exp ð54Þ
RT
T G RT

45:5 !
e_ ¼ 1:5 104 ½sinhð0:05758rÞ 5:9 exp ð52Þ G s 10:21 85:5 9:73 103 ðs=GÞ
RT e_ ¼ 3:23 10 32
exp
T G RT
!
e_ ¼ 7:2 105 ½sinhð0:05728rÞ 6:3 exp
48:0
ð53Þ G s 7:7 115 1:02 104 ðs=GÞ
RT þ 6:93 1029 exp ð55Þ
T G RT
In Sn-3.5Ag solder, Ti and Cd can refine the Ag3Sn particles.
The creep rupture times of Sn-3.0Ag-0.5Cu solder and Sn-3.0Ag-
Moreover, CdSn1.9 particles can be observed in the matrix [175].
0.5Cu-xSnO2 (x = 0.1, 0.5, 1.0 wt%) solder in as-cast condition [160]
The creep resistance of Sn-3.5Ag-0.27Ti and Sn-3.5Ag-0.27Cd show
were investigated indicating that Sn-Ag-Cu solder bearing SnO2
higher value than that of Sn-3.5Ag solder. The Sn-3.5Ag-0.27Cd
nanoparticles exhibits longer creep rupture lives than the original
represents obvious superiority. In Sn-0.7Cu solder, Ag and In can
Sn-Ag-Cu solder. Moreover, with the increase of SnO2 nanoparti-
increase the creep resistance [196]. In Sn-0.7Cu-0.2In solder, the
cles, the creep rupture lives of Sn-Ag-Cu solders can be increased
Ag3Sn and SnIn4 particles can result in impeding the dislocation
significantly. Moreover, the power-law creep model has been used
movement more efficiently, which can decrease the creep rate.
to describe the creep behavior of Sn-3.0Ag-0.5Cu-xSnO2 (x = 0, 0.1,
The increased creep resistance of Sn-0.7Cu-0.2Ag is mostly attrib-
0.5, 1.0 wt%) solders as shown in Eq. (56)-Eq. (59), respectively. The
uted to the attractive interaction between dislocation and Ag3Sn
ZnO nanoparticles have been proved to enhance the creep resis-
particles. The 1.5 wt% Ag and 0.7 wt% Cu elements as additives
tance of Sn-0.7Cu solder [205], and the dislocation pipe diffusion
can also increase the creep resistance of Sn-9Zn solder [217].
was considered as the predominant creep mechanism. The addi-
When metal particles (Ag, Al, Mo, Ni, CuZnAl) and non-metal
tion of Cu6Sn5 nanoparticles into Sn-58Bi solder can induce the
nanoparticles (SnO2, ZnO, Cu6Sn5, CNTs, GNSs) were added into
modification of creep performance [253] with nanoindentation
Sn-Ag-Cu, Sn-Ag, Sn-Cu, Sn-Zn, Sn-Bi lead-free solders, which can
tests. With the increasing of Cu6Sn5 content, the penetration depth
enhance the creep resistance of solders. The Ag nanoparticles
can be reduced, and the creep resistance also can in enhanced
was added into Sn-0.7Cu solder [293], 1.0 vol% Ag particles can
progressively.
effectively prevent dislocation movement and grain boundary dif-
fusion, so the creep rupture life of Sn-Cu solder joints can be e_ ¼ Ar4:8 ð56Þ
increased remarkably. The creep constitutional equations of Sn-
Cu-Ag solder and Sn-Cu solder were established as shown in Eq. e_ ¼ Ar5:4 ð57Þ
(54) and Eq. (55). The Al nanoparticles as additives can prolong
the creep rupture life of Sn-3.8Ag-0.7Cu solder joints [156]. The e_ ¼ Ar5:6 ð58Þ
optimal content of Al nanoparticles was demonstrated to be
0.1 wt%. The effect of the addition of nano-Mo and nano-Ni parti-
e_ ¼ Ar5:7 ð59Þ
cles on the creep behavior of Sn-3.5Ag lead-free solders using a
constant load method in a nanoindenter [179] has been investi- where e_ is the minimum creep rate; A is a material constant.
gated. With the increase of nano-Mo and nano-Ni particle content, During nanoindentation testing, the creep property of Sn-3.5Ag-
primary creep stage displacement. The steady-state creep rate and 0.7Cu solder bearing Ni-coated multi-walled carbon nanotubes
42
(MW-CNTs) was investigated Khodabakhshi [294]. Ni-coated MW- temperature from 55 °C to 125 °C was proposed to evaluate the
CNTS as additives can reduce the indentation depth to enhance the reliability of lead-free solder joints in electronic devices, and the
creep resistance of Sn-Ag-Cu solder, which can be attributed to duration of a thermal cycle is 60 min, including 15 min dwell at
pining action of Ni-coated NW-CNTs on restricting the migration 55 °C and 125 °C. The thermal cycling loading was used in finite
and coalescence of grains. In Han’s work [295], the Ag element analysis. In order to utilize the thermal shock test for reli-
nanoparticles-modified graphene nanosheets (Ag-GNSs) were ability, 40 to 25 °C in compliance with JESD22-A104 condition G
added into Sn-3.0Ag-0.5Cu solder. the GNSs can decrease the isused to evaluate the reliability of solder with 55 °C/min ramp rate
indentation area, which demonstrates that the solders are difficult and more than 12 min dwell time.
to deform due to the addition of Ag-GNSs. With the increase of Ag- It was well demonstrated that creep plays a very important role
GNSs content, the creep resistance can be improved exception of in the deformation behavior of lead-free solders at homologous
0.2 wt%. Moreover, the modified constitutive model for Sn-3.0Ag- temperatures close to and above 0.5 if the loading rate is slow
0.5Cu and Sn-3.0Ag-0.5Cu-0.1Ag-GNSs solders established are as enough for creep deformations to occur [304]. The creep response
follows: may be considered as the main deformation of solder joints in ser-
qffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi2 vice. In the finite element code, the Garofalo-Arrhenius model has
e_ ¼ b r ðrdislocation Þ2 þ rfinegrain 2 þ ðrOrowanIMCs Þ2 ð60Þ been used extensively to describe the steady-state creep of lead-
free solders [305].
Fig. 49 shows the finite element model and stress-strain
qffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi2
response of lead-free solder in 3D structure [303]. The 3D 20-
e_ ¼ b r ðrdislocation Þ2 þ rfinegrain 2 þ ðrOrowanIMCs Þ2 þ rgraphene 2
node structural unit solid 186 is selected to discretize the 1/4 finite
ð61Þ element model. The model is simplified to chips, IMC joints, Sn-Ag-
Cu solder joints, and FR-4 substrates. The stress distribution is not
uniform, and the high-stress region can be found between the chip
6. Reliability of lead-free solder joints and the IMC joints. Since the linear expansion coefficient of the
IMC joints is 23.0 106 K1, and the linear expansion coefficient
6.1. Fatigue reliability of lead-free solder joints in devices of the silicon chip is 2.5 106 K1. The linear expansion coeffi-
cients of the two structures differ greatly, so the volume shrinkage
To evaluate electronic devices, accelerated thermal cycling tests is seriously mismatched during the thermal cycle, and the stress
are often utilized to speed up the thermal fatigue failure process concentration is formed. The maximum stress is concentrated at
assess the reliability of lead-free solder joints under cyclic temper- the lower surface of the corner IMC joint in contact with the chip.
ature variation. According to the thermal cycling testing [303], According to the target characteristics of the design (the expected
Fig. 49. Finite element model and stress-strain response of lead-free solder in 3D structure: (a) 1/4 finite element model of the 3-D package; (b) left view of 1/4 finite element
model; (c) von Mises stress distribution of the 3-D package; (d) S/N response diagram [303].
43
value is as small as possible), the S/N formula based on the small 0.6 lm/s. It is found that with the decrease of IMC thickness at Cu/
characteristic is adopted [306]: Sn-Ag-Cu/Cu solder joints, the smaller value of von Mises demon-
! strated that the more reliability of lead-free solder joint in 3D
1X n
structure.
S=N ¼ 10log y2 ð62Þ
n i¼1 i To improve the reliability of lead-free solder joints in different
devices, the alloying elements can be incorporated into Sn-Ag-Cu
where n is the number of tests; the numerical simulation virtual
solder joints. With the addition of 0.8 wt% Zn, 0.8 wt% Co and
test is used in the paper; so n = 1. yi is the experimental value, which
0.8 wt% Fe, the microstructures and properties of Sn-Ag-Cu solders
is the maximum von Mises stress value r obtained by numerical
can be enhanced remarkably [309]. The Anand constitutive model
simulation.
was investigated under uniaxial tension. Moreover, WLCSP144,
Therefore, Eq. (62) can be written as
WLCSP64, and WLCSP30 devices with Sn-Ag-Cu-Zn, Sn-Ag-Cu-Fe,
S=N ¼ 10log Dr2 ð63Þ and Sn-Ag-Cu-Co solder joints were analyzed using finite element
code. The von Mises stress occurs at the edge of the same solder
According to the S/N response diagram, the contribution degree joint that located on the diagonal of the WLCSP devices as shown
of the four factors is Factor B (solder joint array) > Factor A (IMC in Fig. 50. The maximum stress occurs at the edge area of solder
joint material) > Factor D (substrate thickness) > Factor C (chip joint which is farthest from the center of the device, and this solder
thickness). The most important factor is the solder joint array. In joint is then defined as the key solder joint that is the easiest to be
addition, the IMC joint material also plays an important role in failed under thermal cycling. The addition of Zn, Co, and Fe can
the von Mises stress of solder joints. The thickness of the chip reduce the von-Mises stress and strain in the solder joints. With
and the substrate has little effect on the stress of the solder joints the Engelmaier modified fatigue equation as shown in Eq. (64),
in the 3D package. The optimal parameters match is A2B3C3D3, the fatigue lives of Sn-Ag-Cu-Zn, Sn-Ag-Cu-Fe, and Sn-Ag-Cu-Co
that is, the solder joint array is 2 2 3. The IMC joint material solder joints are higher than that of Sn-Ag-Cu solder joints, which
is Sn3.9Ag0.6Cu. The chip height is 0.2 mm, and the substrate can be attributed to the reduction of the fatigue damages and the
height is 0.35 mm. The optimal parameter design is 69.96% lower change of microcrack propagation site during the fracture process
than the original parameter design. Based on the optimization due to the refinement effect of Zn, Fe, and Co addition.
design and finite element simulation, the reliability of solder joints !1=c
can be evaluated easily. The reliability of Sn-3.0Ag-0.5Cu solder 1 Dc
joints in flip-chip, and the results show the von Mises stress is Nf ¼ 0 ð64Þ
2 2ef
highest at the solder joints at the edge of the device [307]. Cu Core
can be placed on the center of the solder joints to reduce the stress, 0.1 wt% Al nanoparticles can also enhance the reliability of Sn-
and to enhance the reliability of Sn-Ag-Cu solder joints. The Sn-Ag- 3.8Ag-0.7Cu solder joints [310]. The creep performance of Sn-Ag-
Cu solder has been utilized as 3D interconnect materials [308]. The Cu and Sn-Ag-Cu-Al were investigated based on creep testing, as
growth rate of IMC layer during TLP bonding was calculated to be shown in Fig. 51(a). With the addition of 0.1 wt% Al nanoparticles
Fig. 50. Stress distribution of solder joints: (a) Von Mises stress distribution, (b) and (c) Von Mises Stress distribution 3D bars [309].
44
Fig. 51. Creep behavior of lead-free solders: (a) Sn-Ag-Cu and Sn-Ag-Cu-Al and (b) Sn-Ag-Cu and Sn-Ag-Cu-CNT [310].
into Sn-Ag-Cu solder, the creep strain can be decreased signifi- Dx n

Nf ¼A ð67Þ
cantly, so the creep rupture time of Sn-Ag-Cu-Al solder is higher aT þ b
than that of Sn-Ag-Cu solder. The Garofalo-Arrhenius creep model
where a, b, c, and d are the coefficients related to the temperature
was determined to obtain the parameters of both solders. The fati-
effect; m and n are the fatigue exponents; C and A are fatigue duc-
gue life equation as shown in Eq. (65) [304] based on accumulated
tility coefficients; DeP is the plastic strain range in the stabilized
creep strain can be used to calculate the life of solder joints in
cycle; Dx is the inelastic strain energy density in the stabilized
WLCSP device. The fatigue life of Sn-Ag-Cu-Al solder joints can
cycle; Nf is the total number of cycles to failure.
be improved significantly compared with Sn-Ag-Cu solder joints,
Sb is attracting interest as an addition to solders to improve the
and the increased amplitude is 41.9%. The interactions of the dislo-
thermal cycling performance in harsher conditions. The
cations with Al nanoparticles can slow down the climb of disloca-
microstructure evolution and failure of Sn-3.8Ag-0.9Cu-5.5Sb sol-
tion, which can decrease the creep resistance of Sn-Ag-Cu solder
der joint in PBGA device were investigated by Belyakov [314].
joints. With the addition of CNTs, the properties of Sn-Ag-Cu solder
The SbSn particles precipitated preferentially on Cu6Sn5, which
joints can be improved remarkably [311]. The creep parameters of
can improve the reliability of solder joints in harsher accelerated
the Dorn model were determined based on creep testing, and the
thermal cycling. Fig. 52 shows the region containing differing
model was incorporated into finite element code for computing
levels of localized damage in Sn-Ag-Cu-Sb solder joint. In the
the stress-strain response of Sn-Ag-Cu and Sn-Ag-Cu-CNT solder
stress-localized area, larger SbSn particles tend to aggregate at
joints in FCBGA device. The creep strain history of both solder
the recrystallized Sn grain boundaries to prevent the propagation
joints was shown in Fig. 51(b). The creep strain of Sn-Ag-Cu-CNT
of the crack. Finite element simulation was used to analyze the
is lower than that of Sn-Ag-Cu solder joint, which can be attributed
reliability of lead-free solder joints in CSP devices under thermal
to the improvement of creep resistance with the addition of
cycling based on Garofalo-Arrheninus [315]. It is found that the
0.04 wt% CNTs.
Sn-Ag-Cu solders show lower von Mises stress and equivalent
0 1
creep strain than Sn-Ag solder and Sn-Zn solder. The creep strain
Nf ¼ C eacc ð65Þ
distribution has been shown in Fig. 53. Hong [316] proposed the
The effect of Bi as an additive on the mechanical reliability of Eq. (68) and Eq. (69) be utilized in the evaluation of the reliability
Sn-3.0Ag-0.5Cu solder under different loading and aging was of lead-free solder joints based on the fatigue life of traditional Sn-
investigated by Athamneh [312]. It is noted that the addition of Pb solder joints, demonstrating the longer fatigue life of Sn-Ag-Cu
Bi can enhance the fatigue life of Sn-Ag-Cu solder regardless of than that of Sn-Ag and Sn-Zn.
the aging and stress condition. Sn-Ag-Cu-Bi solder joints have a C
higher fatigue resistance and shear strength than Sn-Ag-Cu solder N50 ¼ BI Dein
eq ð68Þ
joints. Based on the microstructure investigation, more precipi-
tates’ coarsening after soldering for Sn-Ag-Cu solder joints can be " #C
N50 ðlead freeÞ eq ðlead freeÞ
Dein
observed compared with Sn-Ag-Cu-Bi solder joints. In Tao’ work ¼ ð69Þ
[313], the Ni, Bi, and Sb were coupling added into Sn-3.8Ag-
N50 ðSn37PbÞ Deineq ðSn37PbÞ
0.7Cu. The low-cycle fatigue testing of series of lead-free solders

where N 50 is the fatigue life; BI and C are the constants of materials;
was conducted using miniature-sized fatigue samples at different
temperature and strain amplitudes. The modified Coffin-Manson
eineq is the single cycle cumulative creep strain; N50 ðlead freeÞ is the
model (Eq. (66)) and modified Morrow model (Eq. (67)) with con- fatigue life of lead-free solder joints; N ðSn37PbÞ is the fatigue life of
Sn-37Pb solder joints; Dein eq ðlead freeÞ and Deeq ðSn37PbÞ are the
in
sideration of the temperature effect were utilized to compute the
fatigue life of lead-free solders, showing that Sn-Ag-Cu-Bi-Sb-Ni creep strain of lead-free solder joints and Sn-37Pb solder joints,
solder has a higher fatigue life than Sn-Ag solder and Sn-Ag-Cu sol- respectively.
der, which demonstrates that the addition of alloying elements can Rare earth Ce can also enhance the reliability of Sn-3.8Ag-0.7Cu
improve the fatigue resistance of lead-free solders. solder joints in WLCSP device [317]. Sn-Ag-Cu-0.03Ce and Sn-Ag-
Cu solder joints in WLCSP were analyzed to calculate the fatigue
DeP m
Nf ¼C ð66Þ life of solder joints. Based on finite element simulation, the
cT þ d stress-strain of Sn-Ag-Cu-Ce solder joints is lower than that of
45
Fig. 52. A region containing differing levels of localized damage in Sn-Ag-Cu-Sb solder joint: (a) BSE image; (b) EBSD map; (c) IPF-X map of Sn and (d) Misorientation of Sn
[314].
Fig. 53. Creep strain of lead-free solder joints array [315].
46
Sn-Ag-Cu solder joints. Moreover, the creep-fatigue life of Sn-Ag- 6.2. Drop reliability of lead-free solder joints
Cu-Ce solder joints is higher than that Sn-Ag-Cu solder joints.
The fatigue life of solder joints is increased by 30.2% with the addi- The reliability assessment of lead-free solder joints under drop
tion of Ce, which can be attributed to the new CeSn3 particles tests is an important method in the electronic industry [323]. So
formed in the matrix resisting the motion of dislocation and the the drop reliability of lead-free solder joints should be conducted
refinement of microstructure. Moreover, with the addition of Al systematically. In Gu’work [324], for analysis of the drop life of
nanoparticles into Sn-3.8Ag-0.7Cu solder joints in FCBGA device. Sn-3.0Ag-0.5Cu solder joints, considering the stress distribution,
The stress-strain response of solder joints can also be improved the drop life prediction model is proposed using a power law for
significantly [318]. It is demonstrated that the stress-strain of Sn- the relationship between the drop life and the drop impact accel-
3.8Ag-0.7Cu-0.1Al solder joints is lower than that of Sn-3.8Ag- eration as Eq. (70). To enhance the drop reliability, the Pb was
0.7Cu solder joints, which demonstrates that the addition of nano added in ENIG surface finish [325]. In the ENIG board, the crack
Al particles can enhance the reliability of Sn-Ag-Cu solder joints. occurs inside the P-rich Ni layer. In ENEPIG board, the crack can
0.1 wt% La2O3 nanoparticles are selected as the additives into Sn- be found inside the inner part of the solder, so the drop reliability
3.8Ag-0.7Cu solder joints for further improve the property during can be improved. Zn was added into Cu layer can also enhance the
thermal cycling loading [56]. The crack can be found between Cu6- drop reliability of Sn-4.0Ag-0.5Cu solder [326]. The Zn can reduce
Sn5 and Cu3Sn as shown in Fig. 54. The crack of Sn-Ag-Cu-La2O3/Cu the growth rate of IMC, suppress the large Ag3Sn and the roughness
solder joints is shorter than that of Sn-Ag-Cu/Cu solder joints, of the interface. Due to modified interfacial microstructure, the
showing that the addition of La2O3 nanoparticles can reduce the drop reliability of solder joints can be improved obviously.
crack length in Sn-Ag-Cu solder joints, which can be attributed to
the thin IMC thickness due to the addition of La2O3 nanoparticles N ¼ C 1 AC 2 ð70Þ
with absorbing effect.
TiO2 nanoparticles can enhance the reliability of Sn-1.0Ag-0.5Cu where N is the drop life of solder joint; A is the impact acceleration;
solder [319]. The microstructure, coefficient of thermal expansion C 1 (6.672) and C 2 (-4.461) are the correlation constants for Sn-Ag-
(CTE), and shear strength of Sn-1.0Ag-0.5Cu solder joints under Cu solder.
thermal cycling (55 to 125 °C). After thermal cycling loading, The reliability and failure analysis of Sn-Ag-Cu and Sn-Ag-Cu-Ni
the 6 nm TiO2 nanoparticles show obvious microstructure refine- lead-free solder joints during drop test were investigated by Wu
ment, CTE reduction, and shear strength enhancement of Sn-Ag- [327]. To improve the reliability evaluation of solder joints under
Cu solder joints. Moreover, the higher electrical reliability than the drop test conditions, Eq. (71) was developed using a power-
Sn-Ag-Cu solder joints can be observed. Al2O3 nanoparticles can law equation. During the drop, the Sn-Ag-Cu based solder joints
also keep higher shear strength of Sn-3.0Ag-0.5Cu-0.06Ni-0.01Ge are subjected to local bending moment, tension, and compression
solder joints during thermal cycling (55 to 125 °C) on as shown in Fig. 55. Four failure modes can be found. Based on
uncoated-Cu or Ni-P coated-Cu [320]. Based on Weibull distribu- the fatigue life prediction of both solder joints, it is demonstrated
tion analysis, the reliability of Sn-Ag-Cu-Ni-Ge solder joints can that the Sn-Ag-Cu-Ni solder joints show higher fatigue life than
be significantly enhanced with the addition of Al2O3 nanoparticles. Sn-Ag-Cu solder joints, which declares that a small amount of Ni
Thermal fatigue reliability of Sn-58Bi solder with the addition of can enhance the fatigue life of Sn-Ag-Cu solder joints.
Ag-decorated MWCNT for LED package component was investi-
N10% ¼ ArBz ð71Þ
gated by Park [321]. During aging (85 °C), the bonding strength
of Sn-Bi based solder joints can be decreased, and the electrical Where N 10% is the number of drops to failure for a 10% failure rate;
resistance can be increased with the increase of aging time. The rZ is the maximum peeling stress in the critical solder joints; A and
formation of the net structure of Ag-MWCNTs can play as the elec- B are the correlation constants.
trical path in the matrix. The electrical and thermal resistance of Until now, the research about drop reliability of new lead-free
the Sn-Bi solder joints reveal the lowest resistance with 0.1 Ag- solders is relatively few, and the influence mechanism of allying
MWCNTs and 0.05 Ag-MWCNTs after aging with 1000 h. For Sn sol-
der, the addition of 0.6% SiC nanowires can impede the IMC growth
and promote the reliability of solder joints with fewer cracks dur-
ing thermal cyclic loading [322], which further demonstrates the
effective influence of nanowires on solders.
Fig. 54. Crack between Cu6Sn5 and Cu3Sn [56]. Fig. 55. Schematic of solder joints failure modes [327].
47
elements and nanoparticles on the drop reliability needs to be fur- bility is an important study in evaluating the applicability of solder
ther studied systematically. in electronic devices.
6.3. Bending reliability of lead-free solder joints 6.4. Electromigration of lead-free solder joints
Bending testing is also an important research method to evalu- Electromigration is one of the most critical reliability problems
ate the reliability of lead-free solder joints in electronic devices. An in the electronic industry and is the main cause of defects in semi-
[328] has studied the mechanical behavior of solder joints under conductor interconnection. The study of electron migration is also
dynamic four-point impact bending, demonstrateing that the an important topic in the field of electronic packaging and testing,
equivalent plastic strain calculated based on rate-dependent and its mechanism and suppression methods have been studied.
Johnson-Cook material model can be utilized to predict failure of The addition of Bi and In into Sn-0.3Ag-0.7Cu solder joints was
solder joints in dynamic bending tests. The finite element simula- studied by Li [331]. The electromigration behavior of solder joints
tion and experiments can be used to analyze the bending reliability was investigated to determine the influence mechanism. Under
of solder joints. electric current with high density, the metal atoms are forced to
For Sn-58Bi solder bearing Sn-MWCNT [134], the three-point move from cathode to anode. The atoms migrating will be
bending test was carried out to assess the reliability of Sn-Bi based increased rapidly, inducing the atoms accumulation at the inter-
solders. Fig. 56 shows the synthesis of Sn-decorated MWCNT face to coarse the IMCs. Due to the addition of Bi and In, at the
nanoparticles with a polyol method designed test-kit for bending interface of Sn-Ag-Cu-Bi-In solder joints, the IMCs layer are Cu6Sn5
test and the illustration of the three-point bending test. For Sn-Bi and Cu6(Sn, In)5. Bi exists in the form of a single substance and
solder joints, after bending test, the cracks propagate through the solid solution to form solid-solution strengthening. Bi and In can
solder joint. For Sn-Bi-0.1MWCNT, the mechanical property can reduce the IMC thickness obviously, which can improve the elec-
be improved obviously, crack after bending test propagates tromigration reliability of Sn-Ag-Cu solder joints.
throughout the interface of solder joint and electrode. For Sn-Bi- The effects of 2.0 vol% Cu particles as additives into Sn-3.5Ag
0.2MWCNT solder joints, due to the aggregation of MWCNTs in solder on electromigration was studied by the in situ process
the matrix, the voids forming during bending the cracks propagate [332]. The retardation of the electromigration phenomenon can
through the voids, which will accelerate the crack propagation. be demonstrated, the growth rate of IMC at the anode decreases
Based on bending experiments, the bending cycles to failure of 73% compared with that of Sn-Ag solder joints after electric current
Sn-58Bi solder bearing 0.1% Ni-MWCNTs can be enhanced obvi- stressing for 528 h. More than three times slower than that of Sn-
ously [329]. For LGA and BGA structures, the bending cycles to fail- Ag solder joints, and no obvious change at the cathode. Cu particles
ure can be improved from 461 to 593 cycles, and 1053 to 1378 can mitigate the polarization effect, and reduce the number of Cu
cycles, respectively. atoms to participate in the interfacial reaction. Ag nanoparticles
For the Sn-3.0Ag-0.5Cu solder with the addition of graphene added into the Sn-58Bi solder joint have been found with enhanced
oxide (GO) powder [330]. The cyclic bending reliability can be electromigration reliability [122]. With the addition of Ag nanopar-
enhanced, and the bending life of Sn-Ag-Cu-0.2GO can be increased ticles, the Ag-Sn IMC particles can be formed to decrease and pre-
by 20% greater than that without Go. In Tian’work [93], the In can vent the IMC growth and the migration of Bi atoms towards the
improve the bending reliability of Sn-0.7Cu solder joints. With In anode, and the electromigration-induced atomic flux of Bi can be
addition, the maximum bending load is higher than that of the calculated using Eq. (72) and Eq. (73). W nanoparticles mitigate
original Sn-Cu solder joints, and the interfacial crack can be sup- the segregation of the Bi-rich and Sn-rich phase remarkably. The
pressed effectively. For a series of lead-free solders, bending relia- addition of W nanoparticles can retard the migration of Au signif-
Fig. 56. Solder and bending: (a) Synthesis process of Sn-decorated MWCNT composite solder; (b) Design of bending test and (c) Three-point bending test [134].
48
icantly, no cathode (Au, Ni)(Sn, Bi)4 layer can be observed, so the (1.38 1023 J/K); T is the temperature; e is the electron charge
addition of W nanoparticles can improve the electromigration (1.6 1019 C), and j is the current density (5 103 A/cm2)
resistance of the Sn-57.6Bi-0.4Ag solder joints [245]. The addition of graphene oxide can influence of electromigra-
tion life of Sn-3.0Ag-0.5Cu solder joints [333]. The electromigration
D Z life of solder increases as the amount of added graphene oxide
J em ¼ C eqj ð72Þ
kT powders increased. With the addition of 0.1 wt% graphene oxide,
So the product of D and Z can be described as follows: the average life increases by 30%. 0.2 wt% graphene oxide can dou-
ble the average life compared with the original Sn-Ag-Cu solder
J em kT joints. The average life of Sn-Ag-Cu, Sn-Ag-Cu-0.1GO, Sn-Ag-Cu-
D Z ¼ ð73Þ
Ceqj 0.2GO solder joints are shown in Fig. 58. Al2O3 nanoparticles added
into Sn-58Bi solder can enhance electromigration reliability. After
where C, D and Z are the concentration, diffusivity, and effective an electromigration test under a current density of 5 103 A/
charge number of the diffusing samples of Bi; q is the resistivity cm2 at 85 °C, the Al2O3 nanoparticles can reduce the thickness of
of the Sn-Bi solder (30 106 Xcm); k is the Boltzmann’s constant the Bi-rich layer, and make the IMC layer decrease by 8% compared
with the Sn-Bi solder [130].
The electromigration behaviors of Sn-58Bi solder bearing Ag-
coated MWCNTs with OSP finished PCB was investigated by Kim
[334]. Due to the addition of Ag-MWCNTs, the growth of reaction
layers can be suppressed between Sn-Bi solder and substrate. The
mean times to failure for the Sn-Bi solder bearing 0–0.1 wt% Ag-
MWCNTs under a current density of 3000 A/cm2 at 100 °C can be
enhanced significantly. Sn-Bi-0.05Ag-MWCNT shows the longest
mean times to failure and 1.4 times longer life than the Sn-Bi sol-
der. So the addition of Ag-MWCNT can enhance the electrical prop-
erties of Sn-58Bi solder.
6.5. Reliability of solder joints under relative humidity environment
Humidity is an important index, which can affect the reliability

of the electronic device. The environment with high humidity is
easy to cause the failure of electronic products, especially for sub-
strate and conductive adhesive. However, relatively little work has
been achieved in the reliability evaluation of lead-free solder or
Fig. 58. The average life of different solder joints [333]. solder joints under a humidity environment.
Fig. 59. Whiskers in Sn3.8Ag0.7Cu-1.8Ce solders: (a) initial whiskers; (b) needle-type whisker; (c) spoon-type whisker; (d) flower-type whisker [336].
49
The microstructures and mechanical properties of Sn-58Bi sol- containing solder alloy [339]. The reaction was shown in Eq. (74)
der containing Ag-decorated MWCNT under 85 °C/85% relative and Eq. (75). Based on the reaction, the Sn can be squeezed out
humidity environmental conditions were investigated by Min as the whiskers. With the oxidation reaction of the RESn3 phase
[335] for 0–1000 h. The shear strength and fracture energy of Sn- with oxygen, the volume of the RESn3 phase will increase obvi-
Bi-0.1MWCNT can be increased approximately by 13% and 21% ously. So the compressive stress (chemical force) can be formed,
compared with the original Sn-Bi solder, respectively. Due to the and the chemical force is essential for spontaneous whiskers
high temperature and high humidity, the interfacial Cu6Sn5 IMC growth.
layer can grow obviously and the grain sizes become coarse with
4RESn3 þ 3O2 ! 2RE2 O3 þ 12Sn ð74Þ
the time increasing, which will induce the degradation of mechan-
ical properties of Sn-Bi-0.1MWCNT and Sn-Bi solders. The refine- 3
ment effect of MWCNT can lead to the higher mechanical 2RESn3 þ 6H2 O þ O2 ! 2REðOHÞ3 þ 6Sn ð75Þ
2
properties of Sn-Bi-0.1MWCNT than Sn-Bi.
To analyze the whisker growth, the SnAgCu-1.8Ce solder was
selected to investigate the whisker’s growth behavior. Fig. 59(a)
6.6. Whiskers in lead-free solders shows the initial whiskers on the surface of CeSn3 particles. The
surface of the particles becomes much darker in color and rougher,
Rare earth Ce [336], Pr [337], and Nd [338] were selected as the indicating that the CeSn3 particles have been oxidized significantly
additive into Sn3.8Ag0.7Cu solder. The relationships between rare in air. Due to the oxidation, the CeSn3 particles will expand obvi-
earth contents and whisker growth were studied systematically. ously. So the compressive stress can be in incubation, which will
Meanwhile, the growth mechanism of whiskers on the surface of be the driving force to squeeze the Sn atoms in the CeSn3 phase.
Sn-Ag-Cu-Ce solders was analyzed. In addition, different morphology whiskers can be found in the sur-
Since rare earth elements are notable for their high chemical face of the CeSn3 phase, the typical morphologies were needle-
activity, they can much more easily react with the oxygen in the type, spoon-type, and flower type, as shown in Fig. 59(b)-(d). Dur-
air and accelerate tin whisker growth in rare earth element- ing the two days of storage, the needle-type whiskers grow at the
Fig. 60. FIB testing and elemental mapping of NdSn3 phase [338].
50
highest rate among all. The maximum length of needle-type whis- cross-section growth behavior. Moreover, a double compressive
kers is 19 lm. For the high-density device, if the needle-type grows stress zone model is developed to explain the growth of Sn
enough in service, there will be at least one whisker long enough to whisker.
connect the adjacent leads or solder joints of the assembly. It is
possible that when there is a strong electrical field in the narrow pR2 e ¼ 2pRc þ E ð76Þ
gap between the whisker tip and the contact point on the other
lead or solder joint. Just before the tip of the whisker touches the 1 2 2
E¼ pR Lq V ð77Þ
other lead or solder joint, a spark may ignite fire [340], which 2
can fail the device. Based on the optimization of rare-earth content.
It can be demonstrated that the critical value of Ce content is 4c
0.1 wt%, and the Ce content should be controlled below 0.1 wt%
R¼ ð78Þ
2e Lq V 2
in the application of Sn-Ag-Cu-xCe solders in the electronic indus-
try. The trace amount of Ce addition can result in small size CeSn3 where E is the whisker kinetic energy; R is the radius of the whis-
particles, which can not form enough driven force by oxidation of ker; L is the whisker length;c is the surface energy per unit area;
CeSn3 to separate the whiskers. For Sn-Ag-Cu-Nd solder, from the q is the whisker density; V is the whisker growth rate, and e is
observation of Fig. 60, it is can be found that under the region of the strain energy per unit volume.
whisker growth, bulk NdSn3 intermetallic compounds appear. For the Sn-9Zn lead-free solder, a small amount of rare earth Pr
With the sluggish oxidation reaction of NdSn3 intermetallic com- can improve the microstructures and properties of solder or solder
pounds, a plentiful Sn layer can be formed, and continuous com- joints in the electronic device. However, for Sn-Zn solder with the
pressive stress can be produced, which can provide enough Sn addition of 0.7 wt% Pr solder, it is found that the Sn whisker can
and driving force for the growth of long whiskers on the NdSn3 grow in the Zn depletion region at the interface during aging
phase. [342]. It is noted that Sn whiskers grow exclusively from the PrSn3
Rare earth Er can be added into Sn-3.8Ag-0.7Cu solder to phase, and the driving force of Sn whisker growth is the local com-
enhance the performance. The 1.0 wt% Er can rapidly promote pressive stress originating from the volume expansion due to the
the Sn whisker growth of Sn-Ag-Cu solder [341]. The chemical oxidized reaction of PrSn3. But no whisker can be observed in Sn-
reaction between ErSn3 and O2 produces the driving force for the Zn-0.08Pr solder. Moreover, the researchers studied the growth
growth. The whiskers with varied nonconstant cross-sections are behavior of Sn whiskers under different environmental conditions
shown in Fig. 61, and the authors give a new energy formula pro- and found that the Sn-9Zn-0.7Pr solder was exposed under room
posed as Eq. (76)-Eq. (78), which can be used to interpret varied ambiance (25 °C, 55% RH) and thermal cycling loading (720 cycles,
Fig. 61. Sn whisker growth with nonconstant cross-section: (a) Cross-section increased abruptly after 150 °C storage for 20 min; (b) Cross-section decreased abruptly after
150 °C storage for 20 min and (c) Cross-section changed continuously after room-temperature storage for 312 h [341].
51
55 to 125 °C) [343]. Under room ambiance, the needle-like whis- resistance of (Ce, Zn)Sn3 phase to inhibit the growth of Sn whiskers
kers can be observed on the surface of the PrSn3 phase, under ther- [344]. In Xue’work [345], Ga as additive into Sn-Zn-Nd solder, can
mal cycling loading, it is noted that the coarse Sn hillocks are the react with Nd to avoid RE-Sn formation to form GaNd and GaNd3
dominant growth morphology as shown in Fig. 62(a), which IMCs, which will reduce the risk of Sn whisker.
demonstrates that the thermal cycling loading can affect the
r ¼ £ða1 a2 ÞDT ð79Þ
growth behavior of Sn whisker. The thermal mismatch stress
between the Sn-Zn matrix and the PrSn3 phase can be calculated where r is the thermal mismatch; £ is a function of the elastic
using Eq. (79). Without the data of the PrSn3 phase, data of the module of both matrix and IMC inclusion and also of the IMC size
CeSn3 phase can be utilized to replace the PrSn3 phase. Since both and distribution; a1 and a2 are the CTEs of matrix and IMC; DT is
phases are RE-Sn phase. Due to the CTE’s mismatch between RE-Sn the temperature difference.
IMC and Sn-9Zn matrix, circumferential compress stress can be For Sn-58Bi solder, with the addition of 0.5 wt% Ce, the fiber-
computed, which are shown in Fig. 62(b)-(d), and the accumulated like and hillock-like Sn whiskers can be observed on the surface
high compressive stress can provide the driving force for the whis- of oxidized Ce(Bi, Sn)3 phase after air storage at 75 °C [346]. Com-
kers growth. For Sn-8Zn-0.5Ce solder, with the addition of 1 wt% pared with Sn-3.0Ag-0.5Cu-0.5Ce solder, the lower Sn content in
and 2 wt% Bi, the (Ce, Zn)Sn3 phase can be refined which can Ce(Bi, Sn)3 phase than in the CeSn3 phase can be found. The
reduce the appearance of Sn whiskers. In addition, 0.5 wt% Ge as compression stress will cause the formation of Sn hillocks. For
additives into Sn-8Zn-3Bi-0.5Ce solder can enhance the oxidation Sn-0.7Cu-0.05Ni solder, the microstructures and properties of Sn-
Fig. 62. FEA analysis of displacement and tress distribution of Sn-Zn based solder: (a) Bulk solder with cracks on IMC surface; (b) Cross-sectioned 2-D model of the solder; (c)
Stress vector and (d) Displacement vector [343].
52
Cu-Ni-xNd/Cu solder joints were investigated by Zeng [347]. For [5] E. Lillie, P. Sandborn, D. Humphrey, Assessing the value of a lead-free solder
control plan using cost-based FMEA, Microelectron. Reliab. 55 (6) (2015) 969–
Sn-Cu-Ni-0.15Nd/Cu solder joints after 3600 h large amount of
979.
Sn whiskers can be observed on the surface of NdSn3 IMC under [6] S. Xu, A.H. Habib, A.D. Pickel, M.E. McHenry, Magnetic nanoparticle-based
room ambiance, and the main morphology of the Sn whisker is hil- solder composites for electronic packaging applications, Prog. Mater Sci. 67
lock and needle-like. However, for Sn-0.7Cu-0.05Ni solder, the (2015) 95–160.
[7] K. Zeng, K. Tu, Six cases of reliability study of Pb-free solder joints in
optimal content of Nd is 0.05 wt%. Therefore, further research is electronic packaging technology, Mater. Sci. Eng., R 38 (2002) 55–105.
needed to determine whether solder joints have Sn whisker in [8] K.S. Kim, S.H. Huh, K. Suganuma, Effects of intermetallic compounds on
service. properties of Sn–Ag–Cu lead-free soldered joints, J. Alloys Compd. 352 (1-2)
(2003) 226–236.
[9] L. Zhang, C.-W. He, Y.-H. Guo, J.-G. Han, Y.-W. Zhang, X.-Y. Wang,
Development of SnAg-based lead free solders in electronics packaging,
7. Conclusions Microelectron. Reliab. 52 (3) (2012) 559–578.
[10] M. Zhao, L. Zhang, Z.-Q. Liu, M.-Y. Xiong, L. Sun, Structure and properties of
Alloying elements and particles as additives can significantly Sn-Cu lead-free solders in electronics packaging, Sci. Technol. Adv. Mater. 20
(1) (2019) 421–444.
influence the IMC layer growth and matrix microstructure, which [11] L. Zhang, S.-B. Xue, L.-l. Gao, Z. Sheng, H. Ye, Z.-X. Xiao, G. Zeng, Y. Chen, S.-L.
are reviewed systematically. The mechanisms of precipitation Yu, Development of Sn–Zn lead-free solders bearing alloying elements, J.
strengthening and solid solution strengthening have been tried to Mater. Sci.-Mater. Electron. 21 (1) (2010) 1–15.
[12] S. Liu, S.-B. Xue, P. Xue, D.-X. Luo, Present status of Sn–Zn lead-free solders
explain the microstructure evaluation and improvement of bearing alloying elements, J. Mater. Sci.-Mater. Electron. 26 (7) (2015) 4389–
mechanical properties. Moreover, no significant change of the 4411.
melting temperature of lead-free solders, only the undercooling [13] F. Wang, H. Chen, Y. Huang, L. Liu, Z. Zhang, Recent progress on the
development of Sn–Bi based low-temperature Pb-free solders, J. Mater. Sci.-
and melting range indicate variation can determine phase precipi-
Mater. Electron. 30 (4) (2019) 3222–3243.
tations and the properties. The wettability of lead-free solders has [14] F. Yang, L. Zhang, Z. Liu, S. Zhong, J. Ma, L. Bao, Properties and microstructures
been reviewed with the addition of alloying elements and particles. of Sn-Bi-X lead-free solders, Adv. Mater. Sci. Eng. 2016 (2016) 9265195.
[15] Y.i. Li, A.B.Y. Lim, K. Luo, Z. Chen, F. Wu, Y.C. Chan, Phase segregation,
The good wettability can enhance the reliability of the solder
interfacial intermetallic growth and electromigration-induced failure in Cu/
joints. For example, the addition of Cu-CNTs can improve the wet- In–48Sn/Cu solder interconnects under current stressing, J. Alloys Compd.
tability of solders, and the creep performance can also be 673 (2016) 372–382.
enhanced. What’s more, the fatigue life of solder joints bearing [16] J.P. Curtulo, M. Dias, F. Bertelli, B.L. Silva, J.E. Spinelli, A. Garcia, N. Cheung, The
application of an analytical model to solve an inverse heat conduction
CNTs can be enhanced with the 41.9% increase in amplitude. problem: Transient solidification of a Sn-Sb peritectic solder alloy on distinct
Although there is so much literature about microstructures and substrates, J. Manuf. Process. 48 (2019) 164–173.
properties of lead-free solders or solder joints, the research results [17] C. Wu, Experimental investigation on phase equilibria of the partial Sn-based
lead-free solder systems, Xiamen University, 2018.
on the reliability of new lead-free solder joints in an electronic [18] M. Yamamoto, I. Shohji, T. Kobayashi, K. Mitsui, H. Watanabe, Effect of small
device are relatively few, especially for drop reliability and humid- amount of ni addition on microstructure and fatigue properties of Sn-Sb-Ag
ity environment. Finally, the new lead-free solders with particle lead-free solder, Materials 14 (2021) 3799.
[19] K. Shohji, Evaluation of microstructures and mechanical properties of sn-
strengthening have been utilized in the 3D IC field. In chip stacking, 10sb-ni lead-free solder alloys with small amount of ni using miniature size
the solder can be completely transformed to IMCs, and the Sn-Bi specimens, Metals 9 (2019) 1348.
solder and Sn-Ag-Cu solder containing CuZnAl particles have been [20] T. Kobayashi, K. Mitsui, I. Shohji, Effects of Ni addition to Sn–5Sb high-
temperature lead-free solder on its microstructure and mechanical
used to improve the reliability of solder joints in 3D IC.
properties, Mater. Trans. 60 (6) (2019) 888–894.
[21] K. Tatsuya, K. Kyosuke, M. Kohei, S. Ikuo, Comparison of sn-5sb and sn-10sb
alloys in tensile and fatigue properties using miniature size specimens, Adv.
Declaration of Competing Interest Mater. Sci. Eng. 2018 (2018) 1416942.
[22] K. Tatsuya, S. Ikuo, N. Yusuke, Effect of power cycling and heat aging on
The authors declare that they have no known competing finan- reliability and imc growth of Sn-5Sb and Sn-10Sb solder joints, Adv. Mater.
Sci. Eng. 2018 (2018) 4829508.
cial interests or personal relationships that could have appeared [23] G. Ren, I.J. Wilding, M.N. Collins, Alloying influences on low melt temperature
to influence the work reported in this paper. SnZn and SnBi solder alloys for electronic interconnections, J. Alloys Compd.
665 (2016) 251–260.
[24] L. Gao, S. Xue, L. Zhang, Z. Sheng, F. Ji, W. Dai, S.-L. Yu, G. Zeng, Effect of
Acknowledgments alloying elements on properties and microstructures of SnAgCu solders,
Microelectron. Eng. 87 (11) (2010) 2025–2034.
[25] L. Zhang, K.N. Tu, Structure and properties of lead-free solders bearing micro
The present work was carried out with the support of the Natural and nano particles, Mater. Sci. Eng., R 82 (2014) 1–32.
Science Foundation of Jiangsu Province (BK20211351), Distin- [26] S. Tikale, K. Narayan Prabhu, Effect of multiple reflow cycles on the shear
guished Researcher project of Henan Province, and the State Key strength of nano-Al2O3 particles reinforced Sn3.6Ag lead-free solder alloy,
Trans. Indian Inst. Met. 71 (11) (2018) 2855–2859.
Lab of Advanced Welding and Joining, Harbin Institute of Technol- [27] H. Tsukamoto, T. Nishimura, S. Suenaga, S.D. McDonald, K.W. Sweatman, K.
ogy (AWJ-19Z04). Nogita, The influence of solder composition on the impact strength of lead-
free solder ball grid array joints, Microelectron. Reliab. 51 (3) (2011) 657–
667.
Data availability [28] J.H.L. Pang, L. Xu, X.Q. Shi, W. Zhou, S.L. Ngoh, Intermetallic growth studies on
Sn-Ag-Cu lead-free solder joints, J. Electron. Mater. 33 (10) (2004) 1219–
1226.
Data sharing is not applicable to this article as no new data were [29] Z. Liang, X.Y. Fan, C.W. He, Y.H. Guo, Intermetallic compound layer growth
created or analyzed in this study. between SnAgCu solder and Cu substrate in electronic packaging, J. Mater.
Sci.-Mater. Electron. 24 (2013) 3249–3254.
[30] J.P. Koppes, K.A. Grossklaus, A.R. Muza, R.R. Revur, S. Sengupta, A. Rae, E.A.
References Stach, C.A. Handwerker, Utilizing the thermodynamic nanoparticle size
effects for low temperature Pb-free solder, Mater. Sci. Eng., B 177 (2012)
197–204.
[1] K. Suganuma, Introduction to lead-free soldering, Science Press, 2017.
[31] Z. Liang, S.B. Xue, L.L. Gao, G. Zeng, S. Zhong, C. Yan, S.L. Yu, Effects of rare
[2] P. Jin, Y. Qin, Y. Hu, C. Wang, Soldering technique of bronzes excavated from
earths on properties and microstructures of lead-free solder alloys, J. Mater.
Jiuliandun tomb in Hubei province, Trans. Chin. Weld. Inst. 28 (2007) 37.
Sci.-Mater. Electron. 20 (2009) 685–694.
[3] M.A. Fazal, N.K. Liyana, S. Rubaiee, A. Anas, A critical review on performance,
[32] C.M.L. Wu, D.Q. Yu, C.M.T. Law, L. Wang, Properties of lead-free solder alloys
microstructure and corrosion resistance of Pb-free solders, Measurement 134
with rare earth element additions, Mater. Sci. Eng., R 44 (2004) 1–44.
(2019) 897–907.
[33] X. Tu, D. Yi, J. Wu, B. Wang, Influence of Ce addition on Sn-3.0Ag-0.5Cu solder
[4] R. Tian, C. Hang, Y. Tian, J. Xu, Brittle fracture of Sn-37Pb solder joints induced
joints: Thermal behavior, microstructure and mechanical properties, J. Alloys
by enhanced intermetallic compound growth under extreme temperature
Compd. 698 (2016) 317–328.
changes, J. Mater. Process. Technol. 268 (2019) 1–9.
53
[34] L. Zhang, S.B. Xue, G. Zeng, L.L. Gao, H. Ye, Interface reaction between SnAgCu/ [61] T. Fouzder, Y.C. Chan, D.K. Chan, Influence of cerium oxide (CeO2)
SnAgCuCe solders and Cu substrate subjected to thermal cycling and nanoparticles on the microstructure and hardness of tin-silver-copper (Sn-
isothermal aging, J. Alloys Compd. 510 (1) (2012) 38–45. Ag-Cu) solders on silver (Ag) surface-finished copper (Cu) substrates, J. Mater.
[35] N. Zhao, M.L. Huang, Y. Zhong, H.T. Ma, X.M. Pan, Effects of rare earth Ce Sci.-Mater. Electron. 25 (12) (2014) 5375–5387.
addition on the microstructure, wettability and interfacial reactions of [62] M. Qu, T. Cao, Y. Cui, F. Liu, Z. Jiao, Effect of nano-ZnO particles on
eutectic Sn-0.7Cu solder, J. Mater. Sci.-Mater. Electron. 26 (1) (2015) 345– wettability, interfacial morphology and growth kinetics of Sn–3.0Ag–0.5Cu–
352. xZnO composite solder, J. Mater. Sci.-Mater. Electron. 30 (21) (2019) 19214–
[36] L. Zhang, X.-Y. Fan, Y.-H. Guo, C.-W. He, Properties enhancement of SnAgCu 19226.
solders containing rare earth Yb, Mater. Des. 57 (2014) 646–651. [63] Y. Tang, Y.C. Pan, G.Y. Li, Influence of TiO2 nanoparticles on thermal property,
[37] J. Wu, S. Xue, J. Wang, G. Huang, Effect of 0.05 wt.% Pr addition on wettability and interfacial reaction in Sn–3.0Ag–0.5Cu–xTiO2 composite
microstructure and shear strength of Sn-0.3Ag-0.7Cu/Cu solder joint during solder, J. Mater. Sci.-Mater. Electron. 24 (5) (2013) 1587–1594.
the thermal aging process, Appl. Sci. 9 (2019) 3590. [64] Y. Wang, X. Zhao, X. Xie, Y. Gu, Y. Liu, Effects of nano-SiO2 particles addition
[38] L. Gao, S. Xue, L. Zhang, Z. Xiao, W. Dai, F. Ji, H. Ye, G. Zeng, Effect of on the microstructure, wettability, joint shear force and the interfacial IMC
praseodymium on the microstructure and properties of Sn3.8Ag0.7Cu solder, growth of Sn3.0Ag0.5Cu solder, J. Mater. Sci.-Mater. Electron. 26 (12) (2015)
J. Mater. Sci.-Mater. Electron. 21 (9) (2010) 910–916. 9387–9395.
[39] S. Li, Y. Liu, H. Zhang, H. Cai, F. Sun, G. Zhang, Microstructure and hardness of [65] L.M. Yang, Z.F. Zhang, Effects of Y2O3 nanoparticles on growth behaviors of
SAC305 and SAC305-0.3Ni solder on Cu, high temperature treated Cu, and Cu6Sn5 grains in soldering reaction, J. Electron. Mater. 42 (12) (2013) 3552–
graphene-coated Cu substrates, Results Phys. 11 (2018) 617–622. 3558.
[40] Q.K. Zhang, W.M. Long, X.Q. Yu, Y.Y. Pei, P.X. Qiao, Effects of Ga addition on [66] A. Aspalter, A. Cerny, M. Göschl, M. Podsednik, G. Khatibi, A. Yakymovych, Y.
microstructure and properties of Sn-Ag-Cu/Cu solder joints, J. Alloys Compd. Plevachuk, Hybrid solder joints: morphology and shear strength of Sn–3.0
622 (2015) 973–978. Ag–0.5 Cu solder joints by adding ceramic nanoparticles through flux doping,
[41] D.-X. Luo, S.-B. Xue, S. Liu, Investigation on the intermetallic compound layer Appl. Nanosci. 10 (2020) 4943–4949.
growth of Sn–0.5Ag–0.7Cu–xGa/Cu solder joints during isothermal aging, J. [67] M. Zhao, L. Zhang, Z.-Q. Liu, M.-Y. Xiong, L. Sun, N. Jiang, K.-K. Xu,
Mater. Sci.-Mater. Electron. 25 (12) (2014) 5195–5200. Microstructures and properties of SnAgCu lead-free solders bearing CuZnAl
[42] H.M. Chen, C.J. Guo, J.P. Huang, W. Hang, Influence of gallium addition in Sn– particles, J. Mater. Sci.-Mater. Electron. 30 (16) (2019) 15054–15063.
Ag–Cu lead-fee solder, J. Mater. Sci.-Mater. Electron. 26 (7) (2015) 5459– [68] L. Zhang, W.-M. Long, F.-J. Wang, Microstructures, interface reaction, and
5464. properties of Sn–Ag–Cu and Sn–Ag–Cu–0.5CuZnAl solders on Fe substrate, J.
[43] L. Zhang, J.-G. Han, C.-W. He, Y.-H. Guo, Effect of Zn on properties and Mater. Sci.-Mater. Electron. 31 (9) (2020) 6645–6653.
microstructure of SnAgCu alloy, J. Mater. Sci.-Mater. Electron. 23 (11) (2012) [69] G. Chen, An investigation into nano-particulates reinforced SAC305-based
1950–1956. composite solders under electro- and thermo-migration conditions,
[44] B. Gabriella, G. Donatella, D. Simona, N. Rada, Effects of Sb addition on the Loughborough University, 2017.
properties of Sn-Ag-Cu/(Cu, Ni) solder systems, J. Alloys Compd. (2016). [70] H. Wang, X. Hu, X. Jiang, Effects of Ni modified MWCNTs on the
[45] Y. Tang, Y.C. Pang, J.X. Zhan, G.Y. Li, Effects of Sb addition on grain ripening microstructural evolution and shear strength of Sn-3.0Ag-0.5Cu composite
growth at interface of Sn-Ag-Cu-xSb/Cu in wetting reactions, Electronic solder joints, Mater. Charact. 163 (2020) 110287.
Packaging Technology and High Density Packaging (ICEPT-HDP), 2012 13th [71] M. Anuar, R. Adawiyah, Interfacial reaction between SAC305 and SAC405
International Conference on, 2012. lead-free solders and electroless nickel/immersion silver (ENImAg) surface
[46] E. Hodúlová, M. Palcut, E. Lechovič, B. Šimeková, K. Ulrich, Kinetics of finish, Universiti tun Hussein Onn Malaysia (2017).
intermetallic phase formation at the interface of Sn–Ag–Cu–X (X = Bi, In) [72] J.-Y. Park, Y.M. Kim, Y.-H. Kim, Improved drop reliability of Sn-Ag-Cu solder
solders with Cu substrate, J. Alloys Compd. 509 (25) (2011) 7052–7059. joints by Zn addition to a Cu wetting layer, J. Mater. Sci.-Mater. Electron. 26
[47] F. Lin, W. Bi, G. Ju, W. Wang, X. Wei, Evolution of Ag3Sn at (8) (2015) 5852–5862.
Sn3.0Ag0.3Cu0.05CrCu joint interfaces during thermal aging, J. Alloys [73] S.S. Ha, H. Kang, G.R. Kim, S. Pae, H. Lee, Effect of corrosion on mechanical
Compd. 509 (2013) 6666–6672. reliability of Sn-Ag flip-chip solder joint, Mater. Trans. 57 (11) (2016) 1966–
[48] J.-X. Chen, X.-k. Zhao, X.-C. Zou, J.-H. Huang, H.-C. Hu, H.-L. Luo, 1971.
Characterization of Cu3P phase in Sn3.0Ag0.5Cu0.5P/Cu solder joints, Int. J. [74] L. Zhang, L. Sun, Y.-H. Guo, C.-W. He, Reliability of lead-free solder joints in
Miner. Metall. Mater. 21 (1) (2014) 65–70. CSP device under thermal cycling, J. Mater. Sci.-Mater. Electron. 25 (3) (2014)
[49] A.S.M.A. Haseeb, M.M. Arafat, M.R. Johan, Stability of molybdenum 1209–1213.
nanoparticles in Sn-3.8Ag-0.7Cu solder during multiple reflow and their [75] L. Sun, M.H. Chen, L. Zhang, P. He, L.S. Xie, Recent progress in SLID bonding in
influence on interfacial intermetallic compounds, Mater. Charact. 64 (2012) novel 3D-IC technologies, J. Alloys Compd. 818 (2019) 152825.
27–35. [76] W.-H. Chen, C.-F. Yu, H.-C. Cheng, Y.-M. Tsai, S.-T. Lu, IMC growth reaction and
[50] S.L. Tay, A.S.M.A. Haseeb, M.R. Johan, P.R. Munroe, M.Z. Quadir, Influence of Ni its effects on solder joint thermal cycling reliability of 3D chip stacking
nanoparticle on the morphology and growth of interfacial intermetallic packaging, Microelectron. Reliab. 53 (1) (2013) 30–40.
compounds between Sn-3.8Ag-0.7Cu lead-free solder and copper substrate, [77] Q. Zhao, A. Hu, M. Li, J. Sun, Effect of electroplating layer structure on shear
Intermetallics 33 (2013) 8–15. property and microstructure of multilayer electroplated Sn–3.5Ag solder
[51] L. Zhang, J.G. Han, C.W. He, Y.H. Guo, J. Zhang, Effect of thermal cycles on the bumps, Microelectron. Reliab. 53 (2) (2013) 321–326.
interface and property of SnAgCu(nano-Al)/Cu solder joints, J. Mater. Eng. 3 [78] K.N. Tu, H.-Y. Hsiao, C. Chen, Transition from flip chip solder joint to 3D IC
(2014) 40–44. microbump: Its effect on microstructure anisotropy, Microelectron. Reliab. 53
[52] Y. Tang, S.M. Luo, G.Y. Li, Z. Yang, R. Chen, Y. Han, C.J. Hou, Effect of Mn (1) (2013) 2–6.
nanoparticles on interfacial intermetallic compound growth in low-Ag Sn-0.3 [79] T. Luo, Z. Chen, A. Hu, M. Li, P. Li, Study on low-Ag content Sn-Ag-Zn/Cu solder
Ag-0.7 Cu-x Mn solder joints, J. Electron. Mater. 47 (2) (2018) 1673–1685. joints, Microelectron. Reliab. 53 (12) (2013) 2018–2029.
[53] X.Y. Liu, M.L. Huang, N. Zhao, L. Wang, Liquid-state and solid-state interfacial [80] H.T. Lee, Y.F. Chen, A. Schwedt, J. Mayer, Effect of La addition on adhesive
reactions between Sn-Ag-Cu-Fe composite solders and Cu substrate, J. Mater. strength and fracture behavior of Sn–3.5Ag solder joints, Mater. Sci. Eng., A
Sci.-Mater. Electron. 25 (2014) 328–337. 528 (2011) 3630–3638.
[54] L. Bin, Research on the improvement of nano-micro Ni, Co particles on Sn-Cu- [81] N. Zhao, X. Pan, Liquid structure of Sn-Ag-xCu solders and its effect on the
Ag hypoeutectic solder, Chongqing University of Technology, 2012. formation and growth of interfacial Cu6Sn5, J. Mater. Sci. 55 (27) (2020)
[55] S. Chellvarajoo, M.Z. Abdullah, Z. Samsudin, Effects of Fe2NiO4 nanoparticles 13294–13302.
addition into lead free Sn-3.0Ag-0.5Cu solder pastes on microstructure and [82] D. Qu, C. Li, L. Bao, Z. Kong, Y. Duan, Structural, electronic, and elastic
mechanical properties after reflow soldering process, Mater. Des. 67 (2015) properties of orthorhombic, hexagonal, and cubic Cu3Sn intermetallic
197–208. compounds in Sn–Cu lead-free solder, J. Phys. Chem. Solids 138 (2019)
[56] L. Zhang, L.-l. Gao, Interfacial compounds growth of SnAgCu(nano La2O3)/Cu 109253.
solder joints based on experiments and FEM, J. Alloys Compd. 635 (2015) 55– [83] Satyanarayan, K.N. Prabhu, Effect of temperature and substrate surface
60. texture on wettability and morphology of IMCs between Sn–0.7Cu solder
[57] J. Wu, S. Xue, J. Wang, P. Xue, Effect of thermal cycling on interfacial alloy and copper substrate, J. Mater. Sci.-Mater. Electron. 23 (9) (2012) 1664–
microstructure and mechanical properties of Sn-0.3Ag-0.7Cu-(a-Al2O3) 1672.
nanoparticles/Cu low-Ag solder joints, J. Electron. Mater. 48 (7) (2019) [84] K. Nogita, M.A.A. Mohd Salleh, E. Tanaka, G. Zeng, S.D. McDonald, S.
4562–4572. Matsumura, In Situ TEM Observations of Cu6Sn5 Polymorphic
[58] S. Chellvarajoo, M.Z. Abdullah, Microstructure and mechanical properties of Transformations in Reaction Layers Between Sn-0.7Cu Solders and Cu
Pb-free Sn–3.0Ag–0.5Cu solder pastes added with NiO nanoparticles after Substrates, JOM 68 (11) (2016) 2871–2878.
reflow soldering process, Mater. Des. 90 (2016) 499–507. [85] Y.-W. Yen, C.-C. Jao, H.-M. Hsiao, C.-Y. Lin, C. Lee, Investigation of the phase
[59] R. Sun, Y. Sui, J. Qi, F. Wei, Y. He, X. Chen, Q. Meng, Z. Sun, Influence of SnO2 equilibria of Sn-Cu-Au ternary and Ag-Sn-Cu-Au quaternary systems and
nanoparticles addition on microstructure, thermal analysis, and interfacial interfacial reactions in Sn-Cu/Au couples, J. Electron. Mater. 36 (2) (2007)
imc growth of Sn1.0Ag0.7Cu solder, J. Electron. Mater. 46 (7) (2017) 4197– 147–158.
4205. [86] H. Wang, J. Fang, Z. Xu, X. Zhang, Improvement of Ga and Zn alloyed Sn–0.7Cu
[60] F. Che Ani, A. Jalar, A.A. Saad, C.Y. Khor, R. Ismail, Z. Bachok, M.A. Abas, N.K. solder alloys and joints, J. Mater. Sci.-Mater. Electron. 26 (6) (2015) 3589–
Othman, The influence of Fe2O3 nano-reinforced SAC lead-free solder in the 3595.
ultra-fine electronics assembly, Int. J. Adv. Manuf. Technol. 96 (1-4) (2018) [87] M. Hasnine, M.J. Bozack, Effects of ga additives on the thermal and wetting
717–733. performance of Sn-0.7Cu solder, J. Electron. Mater. 48 (6) (2019) 3970–3978.
54
[88] T. Kadoguchi, N. Take, K. Yamanaka, S. Nagao, K. Suganuma, Highly [117] R. Zhang, Y. Tian, C. Hang, B. Liu, C. Wang, Formation mechanism and
thermostable joint of Cu/Ni plating/composite Sn–0.7Cu solder with added orientation of Cu 3 Sn grains in Cu–Sn intermetallic compound joints, Mater.
Cu balls for die attachment in power modules, J. Mater. Sci.-Mater. Electron. Lett. 110 (2013) 137–140.
29 (21) (2018) 18290–18301. [118] M. Xiong, L. Zhang, L. Sun, P. He, W. Long, Effect of CuZnAl particles addition
[89] N Zhao, M.L. Huang, Y. Zhao, H.T. Ma, Effects of rare earth Ce addition on the on microstructure of Cu/Sn58Bi/Cu TLP bonding solder joints, Vacuum 167
microstructure, wettability and interfacial reactions of eutectic Sn-0.7Cu (2019) 301–306.
solder, J. Mater. Sci.-Mater. Electron. 26 (2015) 345–352. [119] C. Zhang, S.-D. Liu, G.-T. Qian, J. Zhou, F. Xue, Effect of Sb content on
[90] J. Shen, Y. Pu, D. Wu, Q. Tang, M. Zhao, Effects of minor Bi, Ni on the wetting properties of Sn-Bi solders, Trans. Nonferrous Met. Soc. China 24 (1) (2014)
properties, microstructures, and shear properties of Sn–0.7Cu lead-free solder 184–191.
joints, J. Mater. Sci.-Mater. Electron. 26 (3) (2015) 1572–1580. [120] S.K. Lin, T.L. Nguyen, S.C. Wu, Y.H. Wang, Effective suppression of interfacial
[91] Y. Lai, X. Hu, Y. Li, X. Jiang, Interfacial microstructure evolution and shear intermetallic compound growth between Sn-58 wt.% Bi solders and Cu
strength of Sn0.7Cu-xNi/Cu solder joints, J. Mater. Sci.-Mater. Electron. 29 substrates by minor Ga addition, J. Alloys Compd. 586 (2014) 319–327.
(13) (2018) 11314–11324. [121] L. Yang, L. Zhu, Y.C. Zhang, S.Y. Zhou, G.Q. Wang, S. Shen, X.L. Shi,
[92] Y.-L. Tseng, Y.-C. Chang, C.-C. Chen, Co effects upon intermetallics growth Microstructure, IMCs layer and reliability of Sn-58Bi solder joint reinforced
kinetics in Sn-Cu-Co/Ni and Sn-Cu-Co/Cu couples, J. Electron. Mater. 44 (1) by Mo nanoparticles during thermal cycling, Mater. Charact. 148 (2019) 280–
(2015) 581–589. 291.
[93] S. Tian, S. Li, J. Zhou, F. Xue, R. Cao, F. Wang, Effect of indium addition on [122] S. Ismathullakhan, H. Lau, Y.-C. Chan, Enhanced electromigration reliability
interfacial IMC growth and bending properties of eutectic Sn–0.7 Cu solder via Ag nanoparticles modified eutectic Sn–58Bi solder joint, Microsyst.
joints, J. Mater. Sci.-Mater. Electron. 28 (21) (2017) 16120–16132. Technol. 19 (7) (2013) 1069–1080.
[94] M.A.A. Hanim, N.M. Kamil, C.K. Wei, T.T. Dele-Afolabi, O.S. Azlina, [123] L. Zhang, L. Sun, Y.-H. Guo, Microstructures and properties of Sn58Bi,
Microstructural and shear strength properties of RHA-reinforced Sn–0.7Cu Sn35Bi0.3Ag, Sn35Bi1.0Ag solder and solder joints, J. Mater. Sci.-Mater.
composite solder joints on bare Cu and ENIAg surface finish, J. Mater. Sci.- Electron. 26 (10) (2015) 7629–7634.
Mater. Electron. 31 (11) (2020) 8316–8328. [124] K.-H. Jung, K.D. Min, C.-J. Lee, S.-B. Jung, Pressureless die attach by
[95] Y. Jing, G. Sheng, G. Zhao, Influence of rapid solidification on microstructure, transient liquid phase sintering of Cu nanoparticles and Sn-58Bi particles
thermodynamic characteristic and the mechanical properties of solder/Cu assisted by polyvinylpyrrolidone dispersant, J. Alloys Compd. 781 (2019)
joints of Sn–9Zn alloy, Mater. Des. 52 (2013) 92–97. 657–663.
[96] J. Chen, H. Zhang, P. Zhang, Z. Yu, Y. Zhang, C. Yu, H. Lu, The Zn accumulation [125] A.K. Gain, L. Zhang, Growth mechanism of intermetallic compound and
behavior, phase evolution and void formation in Sn-xZn/Cu systems by mechanical properties of nickel (Ni) nanoparticle doped low melting
considering trace Zn: a combined experimental and theoretical study, J. temperature tin–bismuth (Sn–Bi) solder, J. Mater. Sci.-Mater. Electron. 27
Mater. Res. Technol 8 (5) (2019) 4141–4150. (1) (2016) 781–794.
[97] Y.-H. Hu, S.-B. Xue, H. Ye, Z.-X. Xiao, L.-l. Gao, G. Zeng, Reliability studies of [126] A.K. Gain, L. Zhang, Interfacial microstructure, wettability and material
Sn-9Zn/Cu and Sn-9Zn-0.06Nd/Cu joints with aging treatment, Mater. Des. 34 properties of nickel (Ni) nanoparticle doped tin-bismuth-silver (Sn-Bi-Ag)
(2012) 768–775. solder on copper (Cu) substrate, J. Mater. Sci.-Mater. Electron. 27 (4) (2016)
[98] M.L. Huang, X.L. Hou, N. Kang, Y.C. Yang, Microstructure and interfacial 3982–3994.
reaction of Sn-Zn-x(Al, Ag) near-eutectic solders on Al and Cu substrates, J. [127] N. Jiang, L. Zhang, Z.-Q. Liu, L. Sun, M.-Y. Xiong, M. Zhao, K.-K. Xu, Influences
Mater. Sci.-Mater. Electron. 25 (5) (2014) 2311–2319. of doping Ti nanoparticles on microstructure and properties of Sn58Bi solder,
[99] W. Chen, S. Xue, H. Wang, J. Wang, Z. Han, Solderability and intermetallic J. Mater. Sci.-Mater. Electron. 30 (19) (2019) 17583–17590.
compounds formation of Sn-9Zn-xAg lead-free solders wetted on Cu [128] X. Qiu, H. Wei, Q. Wang, P. He, F. Lu, Effect of La2O3 particles on structure and
substrate, Rare Met. 28 (6) (2009) 656–660. properties of Sn-58Bi solder after multi-remelting, Mater. Sci. Technol. 23
[100] H. Wang, Study on solderability and wetting mechanisms of micro-alloyed (2015) 20–24.
Sn-9Zn lead-free solder, Nanjing University of Aeronautics and Astronautics, [129] A. Sharma, A.K. Srivastava, K. Lee, B. Ahn, Impact of non-reactive ceria
2010. nanoparticles on the wettability and reaction kinetics between lead-free Sn–
[101] T. Gancarz, P. Bobrowski, S. Pawlak, N. Schell, R. Chulist, K. Janik, Wetting of 58Bi and Cu pad, Met. Mater.-Int. 25 (4) (2019) 1027–1038.
Sn-Zn-Ga and Sn-Zn-Na alloys on Al and Ni substrate, J. Electron. Mater. 47 [130] T. Hu, Y.i. Li, Y.-C. Chan, F. Wu, Effect of nano Al2O3 particles doping on
(1) (2018) 49–60. electromigration and mechanical properties of Sn-58Bi solder joints,
[102] W.X. Chen, S.B. Xue, H. Wang, Wetting properties and interfacial Microelectron. Reliab. 55 (8) (2015) 1226–1233.
microstructures of Sn–Zn– xGa solders on Cu substrate, Mater. Des. 31 (4) [131] X. Liu, M. Huang, C.M.L. Wu, L. Wang, Effect of Y2O3 particles on
(2010) 2196–2200. microstructure formation and shear properties of Sn-58Bi solder, J. Mater.
[103] P. Fima, T. Gancarz, J. Pstru, A. Sypień, Wetting of Sn-Zn-xIn (x=0.5, 1.0, 1.5 wt Sci.-Mater. Electron. 21 (10) (2010) 1046–1054.
%) Alloys on Cu and Ni Substrates, J. Mater. Eng. Perform. 21 (2012) 595–598. [132] C.J. Lee, K.D. Min, H.J. Park, S.B. Jung, Mechanical properties of Sn-58wt%Bi
[104] G. Zhao, G. Sheng, J. Luo, X. Yuan, Solder characteristics of a rapidly solidified solder containing Ag-decorated MWCNT with thermal aging tests, J. Alloys
Sn-9Zn-0.1Cr alloy and mechanical properties of Cu/Solder/Cu joints, J. Compd. 820 (2020) 153077.
Electron. Mater. 41 (8) (2012) 2100–2106. [133] C.-J. Lee, K.D. Min, B.-U. Hwang, J.-H. Kim, S.-B. Jung, The effect of pH on
[105] J.-C. Liu, G. Zhang, Z.-H. Wang, J.-S. Ma, K. Suganuma, Thermal property, synthesizing Ni-decorated MWCNTs and its application for Sn-58Bi solder,
wettability and interfacial characterization of novel Sn-Zn-Bi-In alloys as Curr. Appl. Phys. 19 (11) (2019) 1182–1186.
low-temperature lead-free solders, Mater. Des. 84 (2015) 331–339. [134] C.J. Lee, K.D. Min, H.J. Park, J.H. Kim, S.B. Jung, Effect of Sn-decorated MWCNTs
[106] A. Gain Kumar, L. Zhang, Microstructure, thermal analysis and damping on the mechanical reliability of Sn–58Bi solder, Electron. Mater. Lett. 15
properties of Ag and Ni nano-particles doped Sn-8Zn-3Bi solder on OSP-Cu (2019) 1182–1186.
substrate, J. Alloys Compd. 617 (2014) 779–786. [135] L. Sun, L. Zhang, Properties and Microstructures of Sn-Ag-Cu-X Lead-Free
[107] Y.-W. Yen, W.-K. Liou, W.-C. Chen, C.-W. Chiu, Aging and Cu concentration Solder Joints in Electronic Packaging, Adv. Mater. Sci. Eng. 2015 (2015)
effects on Sn-9Zn-xCu/Au couples, J. Alloys Compd. 574 (2013) 490–494. 639028.
[108] L. Liu, P. Wu, W. Zhou, Effects of Cu on the interfacial reactions between Sn- [136] K.-K. Xu, L. Zhang, L. Sun, N. Jiang, M. Zhao, M.-Y. Xiong, The influence of
8Zn-3Bi-xCu solders and Cu substrate, Microelectron. Reliab. 54 (1) (2014) carbon nanotubes on the properties of Sn solder, Mater. Trans. 61 (4) (2020)
259–264. 718–722.
[109] W.-Q. Xing, X.-y. Yu, H. Li, L.e. Ma, W. Zuo, P. Dong, W.-X. Wang, M. Ding, [137] S.-W. Chen, C.-H. Wang, S.-K. Lin, C.-N. Chiu, Phase diagrams of Pb-free
Effect of nano Al2O3 additions on the interfacial behavior and mechanical solders and their related materials systems, J. Mater. Sci.-Mater. Electron. 18
properties of eutectic Sn-9Zn solder on low temperature wetting and (1-3) (2006) 19–37.
soldering of 6061 aluminum alloys, J. Alloys Compd. 695 (2017) 574–582. [138] K.S. Kim, S.H. Huh, K. Suganuma, Effects of cooling speed on microstructure
[110] Q.J. Zhai, S.K. Guan, Q.Y. Shang, Alloy thermo-mechanism: theory and and tensile properties of Sn-Ag-Cu alloys, Mater. Sci. Eng., A 333 (2002) 106–
application, Metallurgy Industry Press, Beijing, 1999. 114.
[111] R. Sui, F. Li, W. Ci, Q. Lin, Wetting of Cu and Cu-Sn IMCs by Sn-Bi Alloys over [139] L. Gao, S. Xue, L. Zhang, Z. Sheng, G. Zeng, F. Ji, Effects of trace rare earth Nd
Wide Composition at 350°C, J. Electron. Mater. 48 (7) (2019) 4660–4668. addition on microstructure and properties of SnAgCu solder, J. Mater. Sci.-
[112] Y.A. Shen, S. Zhou, J. Li, C.H. Yang, H. Nishikawa, Sn-3.0Ag-0.5Cu/Sn-58Bi Mater. Electron. 21 (7) (2010) 643–648.
composite solder joint assembled using a low-temperature reflow process for [140] L. Gao, S. Xue, H. Xu, Microstructure and properties of SnAgCu-xPr solder,
PoP technology, Mater. Des. 183 (2019) 108144. Trans. Chin. Weld. Inst. 33 (2012) 69–72.
[113] Y.-Y. Shiue, T.-H. Chuang, Effect of La addition on the interfacial [141] L. Zhang, J. Han, Y. Guo, Z. Lai, L. Zhang, Microstructures and property of
intermetallics and bonding strengths of Sn-58Bi solder joints with Au/Ni/ SnAgCu/SnAgCuCe solder joints, Chin. J. Mech. Eng. 48 (2012) 67–73.
Cu pads, J. Alloys Compd. 491 (1-2) (2010) 610–617. [142] A.M. El-Taher, A.F. Razzk, Controlling Ag3Sn plate formation and its effect on
[114] F.Q. Hu, Q.K. Zhang, J.J. Jiang, Z.L. Song, Influences of Ag addition to Sn-58Bi the creep resistance of Sn–3.0Ag–0.7Cu lead-free solder by adding minor
solder on SnBi/Cu interfacial reaction, Mater. Lett. 214 (2018) 142–145. alloying elements Fe Co, Te and Bi, Met. Mater.-Int. 27 (10) (2021) 4294–
[115] D. Ma, P. Wu, Effects of Zn concentration on the aging reactions and IMC 4305.
massive spalling phenomenon in the Sn-58Bi-xZn/Cu system, J. Mater. Sci.- [143] Z.L. Ma, H. Shang, A.A. Daszki, S.A. Belyakov, C.M. Gourlay, Mechanisms of
Mater. Electron. 26 (3) (2015) 1338–1346. beta-Sn nucleation and microstructure evolution in Sn-Ag-Cu solders
[116] L. Zhang, Z.Q. Liu, Inhibition of intermetallic compounds growth at Sn–58Bi/ containing titanium, J. Alloys Compd. 777 (2019) 1357–1366.
Cu interface bearing CuZnAl memory particles (2–6 lm), J. Mater. Sci.-Mater. [144] D.A. Shnawah, M.F.M. Sabri, I.A. Badruddin, S.B.M. Said, T. Ariga, F.X. Che,
Electron. 31 (2020) 2466–2480. Effect of Ag content and the minor alloying element Fe on the mechanical
55
properties and microstructural stability of Sn-Ag-Cu solder alloy under high- [172] S. Liu, W. Xiong, J. Xiong, G. Tan, Z. Hu, C. Chen, S. Huang, Refinement
temperature annealing, J. Electron. Mater. 42 (3) (2013) 470–484. mechanism of Bi addition on the microstructure of rapidly solidified Sn-3.5Ag
[145] M.H. Mahdavifard, M.F.M. Sabri, S.M. Said, S. Rozali, High stability and aging eutectic solder for microelectronic packaging, J. Electron. Mater. 47 (9) (2018)
resistance Sn-1Ag-0.5Cu solder alloy by Fe and Bi minor alloying, 5588–5594.
Microelectron. Eng. 208 (2019) 29–38. [173] M.S. Gumaan, Chromium improvements on the mechanical performance of a
[146] A.A. El-Daly, A.E. Hammad, G.S. Al-Ganainy, M. Ragab, Influence of Zn rapidly solidified eutectic Sn–Ag alloy, J. Mater. Sci.-Mater. Electron. 31 (13)
addition on the microstructure, melt properties and creep behavior of low (2020) 10731–10737.
Ag-content Sn–Ag–Cu lead-free solders, Mater. Sci. Eng., A 608 (2014) 130– [174] W.M. Chen, S.K. Kang, C.R. Kao, Effects of Ti addition to Sn–Ag and Sn–Cu
138. solders, J. Alloys Compd. 520 (2012) 244–249.
[147] Z.-B. Luo, J. Zhao, Y.-J. Gao, L. Wang, Revisiting mechanisms to inhibit Ag3Sn [175] B.A. Khalifa, R.A. Ismail, A.M. Yassin, Structure analysis and enhancement of
plates in Sn–Ag–Cu solders with 1 wt.% Zn addition, J. Alloys Compd. 500 (1) creep resistance and thermal properties of eutectic Sn-Ag lead free solder
(2010) 39–45. alloy by Ti and Cd - addition, J. Adv. Phys. 13 (2017) 5092–5099.
[148] J. Mao, B. Reeves, B. Lenz, D. Ruscitto, D. Lewis, Study on the effect of Mn, Zn, [176] M.S. Gumaan, R.M. Shalaby, M.K. Mohammed Yousef, E.A.M. Ali, E.E. Abdel-
and Sb on undercooling behavior of Sn-Ag-Cu alloys using differential Hady, Nickel effects on the structural and some physical properties of the
thermal analysis, J. Electron. Mater. 46 (11) (2017) 6319–6332. eutectic Sn-Ag lead-free solder alloy, SSMT 31 (1) (2019) 40–51.
[149] X. Kong, J. Zhai, F. Sun, Y. Liu, H. Zhang, Combined effect of Bi and Ni elements [177] A. Nadia, A. Haseeb, Effects of addition of copper particles of different size to
on the mechanical properties of low-Ag Cu/Sn-0.7Ag-0.5Cu/Cu solder joints, Sn-3.5Ag solder, J. Mater. Sci.-Mater. Electron. 23 (1) (2012) 86–93.
Microelectron. Reliab. 107 (2020) 113618. [178] P. Tunthawiroon, K. Kanlayasiri, Effects of Ag contents in Sn–xAg lead-free
[150] A.K. Gain, L. Zhang, Effects of Ni nanoparticles addition on the microstructure, solders on microstructure, corrosion behavior and interfacial reaction with
electrical and mechanical properties of Sn-Ag-Cu alloy, Materialia 2019 Cu substrate, Trans. Nonferrous Met. Soc. China 29 (8) (2019) 1696–1704.
(2019) 100234. [179] V.L. Niranjani, B.S.S. Chandra Rao, R. Sarkar, S.V. Kamat, The influence of
[151] L. Yang, S. Quan, C. Liu, G. Shi, Aging resistance of the Sn-Ag-Cu solder joints addition of nanosized molybdenum and nickel particles on creep behavior of
doped with Mo nanoparticles, Mater. Lett. 253 (2019) 191–194. Sn–Ag lead free solder alloy, J. Alloys Compd. 542 (2012) 136–141.
[152] Y.u. Tang, S. Luo, G. Li, Z. Yang, C. Hou, Effects of Mn nanoparticle addition [180] X. Xia, F. Tai, Effects of processing conditions on microstructures and
on wettability, microstructure and microhardness of low-Ag Sn-0.3Ag-0.7Cu- properties of particulate reinforced composite solder joints, Rare Metal
x Mn(np) composite solders, Solder. Surf. Mt. Technol. 30 (3) (2018) 153–163. Mat. Eng. 40 (2011) 75–79.
[153] A. Yakymovych, S. Mudry, I. Shtablavyi, H. Ipser, Effect of nano Co [181] F. Tai, F. Guo, L. Ma, M. Han, Effects of service conditions on properties of in-
reinforcements on the structure of the Sn-3.0Ag-0.5Cu solder in liquid and situ particle-reinforced composite solder joint, Trans. Chin. Weld. Inst. 31
after reflow solid states, Mater. Chem. Phys. 181 (2016) 470–475. (2010) 81–84.
[154] S.Y. Xu, A.H. Habib, A. Prasitthipayong, M.E. Mchenry, Effects of FeCo [182] Y.-K. Ko, S.-H. Kwon, Y.-K. Lee, J.-K. Kim, C.-W. Lee, S. Yoo, Fabrication and
magnetic nanoparticles on microstructure of Sn-Ag-Cu alloys, J. Appl. Phys. interfacial reaction of carbon nanotube-embedded Sn-3.5Ag solder balls for
113 (2013) 17A301. ball grid arrays, J. Alloys Compd. 583 (2014) 155–161.
[155] L. Zhang, X.-Y. Fan, Y.-H. Guo, C.-W. He, Microstructures and fatigue life of [183] A. Sharma, A.K. Srivastava, B. Ahn, Microstructure, wetting, and tensile
SnAgCu solder joints bearing Nano-Al particles in QFP devices, Electron. behaviors of Sn-Ag Alloy reinforced with copper-coated carbon nanofibers
Mater. Lett. 10 (3) (2014) 645–647. produced by the melting and casting route, Metall. Mater. Trans. A 50 (11)
[156] L. Zhang, J. Han, Y. Guo, C. He, J. Zhang, Microstructures and properties of (2019) 5384–5394.
SnAgCu solders bearing nano-particles Al, Trans. Chin. Weld. Inst. 34 (2013) [184] M. Sobhy, Effects of torsional oscillation on tensile behavior of Sn-3.5 wt% Ag
65–68. alloy with and without adding ZnO nanoparticles, Mater. Sci. Eng., A 610
[157] S.H. Chang, S.K. Wu, C. Kuo, Effect of reinforced multiwall carbon nanotubes (2014) 237–242.
on the damping characteristics of Sn-Ag-Cu lead-free solder, Mater. Lett. 276 [185] A. Sharma, S. Bhattacharya, S. Das, K. Das, Fabrication of Sn-Ag/CeO2 electro-
(2020) 128196. composite solder by pulse electrodeposition, Metall. Mater. Trans. A 44 (12)
[158] D.-H. Jung, A. Sharma, J.-P. Jung, Influence of dual ceramic nanomaterials on (2013) 5587–5601.
the solderability and interfacial reactions between lead-free Sn-Ag-Cu and a [186] F. Tai, F. Guo, Z.D. Xia, Y.P. Lei, Y.W. Shi, Effects of nano-structured particles
Cu conductor, J. Alloys Compd. 743 (2018) 300–313. on microstructure and microhardness of Sn–Ag solder alloy, J. Mater. Sci.-
[159] S.Y. Chang, L.C. Tsao, M.W. Wu, C.W. Chen, The morphology and kinetic Mater. Electron. 21 (7) (2010) 702–707.
evolution of intermetallic compounds at Sn–Ag–Cu solder/Cu and Sn–Ag–Cu- [187] M. Zhao, L. Zhang, M. Xiong, Research status and development trend of Sn-Cu
0.5Al2O3 composite solder/Cu interface during soldering reaction, J. Mater. lead-free solders, Mater. Rep. 33 (2019) 2467–2478.
Sci.-Mater. Electron. 23 (1) (2012) 100–107. [188] Satyanarayan, K.N. Prabhu, Reactive wetting, evolution of interfacial and
[160] A. Wattanakornphaiboon, R. Canyook, K. Fakpan, Effect of SnO2 bulk IMCs and their effect on mechanical properties of eutectic Sn-Cu solder
reinforcement on creep property of Sn–Ag–Cu solders, Mater. Today 5 alloy, Adv. Colloid Interface Sci. 166 (1-2) (2011) 87–118.
(2018) 9213–9219. [189] M. Drienovsky, L.R. Trnkova, M. Martinkovic, M. Ozvold, I. Cernickova, M.
[161] A.K. Gain, Y.C. Chan, W.K.C. Yung, Effect of additions of ZrO2 nano-particles on Palcut, J. Janovec, Influence of cerium addition on microstructure and
the microstructure and shear strength of Sn–Ag–Cu solder on Au/Ni properties of Sn-Cu-(Ag) solder alloys, Mater. Sci. Eng., A 623 (2015) 83–91.
metallized Cu pads, Microelectron. Reliab. 51 (12) (2011) 2306–2313. [190] L. Zhang, S. Xue, Y. Chen, Z. Han, J. Wang, S. Yu, F. Lu, Effects of cerium on Sn-
[162] M. Sobhy, A.M. El-Refai, M.M. Mousa, G. Saad, Effect of ageing time on the Ag-Cu alloys based on finite element simulation and experiments, J. Rare
tensile behavior of Sn-3.5 wt% Ag-0.5 wt% Cu (SAC355) solder alloy with and Earths 27 (1) (2009) 138–144.
without adding ZnO nanoparticles, Mater. Sci. Eng., A 646 (2015) 82–89. [191] G. Zeng, S. Xue, Z.L. Gao, Z. Lai, J. Luo, Properties and microstructure of Sn-
[163] A. Sharma, B.G. Baek, J.P. Jung, Influence of La2O3 nanoparticle additions on 0.7Cu-0.05Ni solder bearing rare earth element Pr, J. Mater. Sci. 22 (2011)
microstructure, wetting, and tensile characteristics of Sn–Ag–Cu alloy, Mater. 1101–1108.
Des. 87 (2015) 370–379. [192] L. Zhang, L. Tian, Y. Guo, L. Sun, Y. Min, Wettability of SnCuNi-xEu solders and
[164] D.-H. Jung, A. Sharma, D.-U. Lim, J.-H. Yun, J.-P. Jung, Effects of AlN mechanical properties of solder joints, J. Rare Earths 32 (12) (2014) 1184–
Nanoparticles on the Microstructure, Solderability, and Mechanical 1188.
Properties of Sn-Ag-Cu Solder, Metall. Mater. Trans. A 48 (9) (2017) 4372– [193] J. Koo, C. Lee, S.J. Hong, K.-S. Kim, H.M. Lee, Microstructural discovery of Al
4384. addition on Sn-0.5Cu-based Pb-free solder design, J. Alloys Compd. 650
[165] A.A. El-Daly, G.S. Al-Ganainy, A. Fawzy, M.J. Younis, Structural (2015) 106–115.
characterization and creep resistance of nano-silicon carbide reinforced Sn– [194] J. Bang, D.-Y. Yu, Y.-H. Ko, M.-S. Kim, H. Nishikawa, C.-W. Lee, Intermetallic
1.0Ag–0.5Cu lead-free solder alloy, Mater. Des. 55 (2014) 837–845. compound formation and mechanical property of Sn-Cu-xCr/Cu lead-free
[166] G. Chen, H. Peng, V.V. Silberschmidt, Y.C. Chan, C. Liu, F. Wu, Performance of solder joint, J. Alloys Compd. 728 (2017) 992–1001.
Sn-3.0Ag-0.5Cu composite solder with TiC reinforcement: Physical [195] B.L. Silva, N. Cheung, A. Garcia, J.E. Spinelli, Evaluation of solder/substrate
properties, solderability and microstructural evolution under isothermal thermal conductance and wetting angle of Sn-0.7 wt%Cu-(0–0.1 wt%Ni)
ageing, J. Alloys Compd. 685 (2016) 680–689. solder alloys, Mater. Lett. 142 (2015) 163–167.
[167] X. Zhao, Y. Wen, Y.i. Li, Y. Liu, Y. Wang, Effect of c-Fe2O3 nanoparticles size on [196] A.A. El-Daly, A.E. Hammad, Enhancement of creep resistance and thermal
the properties of Sn-1.0 Ag–0.5 Cu nano-composite solders and joints, J. behavior of eutectic Sn–Cu lead-free solder alloy by Ag and In-additions,
Alloys Compd. 662 (2016) 272–282. Mater. Des. 40 (2012) 292–298.
[168] T. Fouzder, I. Shafiq, Y.C. Chan, A. Sharif, W.K.C. Yung, Influence of SrTiO3 [197] H.H. Zhen, S.G. Wang, W.X. Qin, Y.C. Qiang, Effects of sulfur addition on the
nano-particles on the microstructure and shear strength of Sn-Ag-Cu solder wettability and corrosion resistance of Sn-0.7Cu lead-free solder,
on Au/Ni metallized Cu pads, J. Alloys Compd. 509 (5) (2011) 1885–1892. Microelectron. Reliab. 74 (2017) 15–21.
[169] A.K. Gain, L. Zhang, Thermal aging effects on microstructure, elastic property [198] L.F. Li, Y.K. Cheng, G.L. Xu, E.Z. Wang, Z.H. Zhang, H. Wang, Effects of indium
and damping characteristic of a eutectic Sn–3.5Ag solder, J. Mater. Sci.-Mater. addition on properties and wettability of Sn–0.7Cu–0.2Ni lead-free solders,
Electron. 29 (17) (2018) 14519–14527. Mater. Des. 64 (2014) 15–20.
[170] W.-Y. Chen, J.-G. Duh, Suppression of Cu3Sn layer and formation of multi- [199] X. Hu, Y. Li, Y.i. Liu, Z. Min, Developments of high strength Bi-containing
orientation IMCs during thermal aging in Cu/Sn–3.5Ag/Cu–15Zn transient Sn0.7Cu lead-free solder alloys prepared by directional solidification, J. Alloys
liquid-phase bonding in novel 3D-IC technologies, Mater. Lett. 186 (2017) Compd. 625 (2015) 241–250.
279–282. [200] K. Kanlayasiri, R. Kongchayasukawat, Property alterations of Sn-0.6Cu-
[171] Q.K. Zhang, Investigations on Microstructure and Mechanical Properties of 0.05Ni-Ge lead-free solder by Ag, Bi, In and Sb addition, Trans. Nonferrous
the Cu/Pb-Free Solder Joint Interfaces, Springer, 2015. Met. Soc. China 28 (6) (2018) 1166–1175.
56
[201] L.i. Yang, J. Ge, Y. Zhang, J. Dai, H. Liu, J. Xiang, Investigation on the [230] W.R. Osório, L.C. Peixoto, L.R. Garcia, N. Mangelinck-Noël, A. Garcia,
microstructure, interfacial IMC layer, and mechanical properties of Cu/Sn- Microstructure and mechanical properties of Sn–Bi, Sn–Ag and Sn–Zn lead-
0.7Cu-xNi/Cu solder joints, J. Electron. Mater. 45 (7) (2016) 3766–3775. free solder alloys, J. Alloys Compd. 572 (2013) 97–106.
[202] W. Yang, Y. Lv, X. Zhang, X. Wei, Y. Li, Y. Zhan, Influence of graphene [231] X. Yu, X. Hu, Y. Li, T. Liu, R. Zhang, Z. Min, Tensile properties of Cu/Sn–58Bi/Cu
nanosheets addition on the microstructure, wettability, and mechanical soldered joints subjected to isothermal aging, J. Mater. Sci.-Mater. Electron.
properties of Sn-0.7Cu solder alloy, J. Mater. Sci.-Mater. Electron. 31 (17) 25 (6) (2014) 2416–2425.
(2020) 14035–14046. [232] X. Chen, Investigation on the microstructure and properties of Sn-Bi based
[203] M.M. Salleh, A.M. Al Bakri, M.H. Zan, F. Somidin, N.F.M. Alui, Z.A. Ahmad, solder alloys, Southeast University, 2017.
Mechanical properties of Sn–0.7Cu/Si3N4lead-free composite solder, Mater. [233] S. Liu, T. Song, W. Xiong, L.i. Liu, Z. Liu, S. Huang, Effects of Ag on the
Sci. Eng., A 556 (2012) 633–637. microstructure and shear strength of rapidly solidified Sn-58Bi solder, J.
[204] A. Mohammadi, R. Mahmudi, Elevated-temperature mechanical properties of Mater. Sci.-Mater. Electron. 30 (7) (2019) 6701–6707.
lead-free Sn-0.7Cu- xSiC nanocomposite solders, J. Electron. Mater. 47 (2) [234] L. Gong, J. Liao, J. Yuan, L.I. Guihe, H. Chen, Effect of Rare Earth Y on
(2018) 1721–1729. Microstructure and Properties of Sn-58Bi Solder Alloy, J. Aeronaut. Mat. 38
[205] A.F. Abd El-Rehim, H.Y. Zahran, A.M. Yassin, Microstructure evolution and (2018) 101–108.
tensile creep behavior of Sn–0.7Cu lead-free solder reinforced with ZnO [235] J. Liao, L. Gong, D. Yuan, D. Wang, H. Chen, Effects of Ce addition on
nanoparticles, J. Mater. Sci.-Mater. Electron. 30 (3) (2019) 2213–2223. microstructure and properties of Sn-58Bi solder alloy, Chin. J. Process Eng. 18
[206] M.A.A. Mohd Salleh, S.D. McDonald, C.M. Gourlay, H. Yasuda, K. Nogita, (2018) 618–623.
Suppression of Cu6Sn5 in TiO2 reinforced solder joints after multiple reflow [236] K. He, Y. Chen, D. Hu, D. Cheng, Z. Li, S. Huang, Y. Guo, Effect of Al element on
cycles, Mater. Des. 108 (2016) 418–428. microstructure and mechanical properties of hypoeutectic SnBi solder joint,
[207] H. Wang, Study on solderability and wetting mechanisms of micro-alloyed Trans. Mat. Heat Treat. 41 (2020) 163–168.
Sn-9Zn lead-free solder, Nanjing University of Aeronautics and Astronautics, [237] X. Wang, B. Liu, H. Zhou, J. Wang, N. Liu, T. Li, Effect of P on Microstructure
2010. and Mechanical Properties of Sn-Bi Solder, J. Mater. Eng. 44 (2016).
[208] W. Chen, Effects of Ag, Ga, Al and Ce on the properties of Sn-9Zn lead-free [238] J.G. Li, X. Ma, M.B. Zhou, X. Ning, X.P. Zhang, Effects of Sb addition on the
solder, Nanjing University of Aeronautics and Astronautics, 2010. microstructure and mechanical performance of Sn58Bi based alloys and the
[209] Z. Xiao, Effect of Pr on the microstructure and properties of Sn-9Zn lead-free solder joints, 2018 19th International Conference on Electronic Packaging
solder, Nanjing University of Aeronautics and Astronautics, 2011. Technology (ICEPT), 2018.
[210] L. Zhang, J. Cui, J. Han, Y. Guo, C. He, Microstructures and properties of SnZn- [239] X. Chen, F. Xue, J. Zhou, Y. Yao, Effect of In on microstructure, thermodynamic
xEr lead-free solders, J. Rare Earths 30 (8) (2012) 790–793. characteristic and mechanical properties of Sn-Bi based lead-free solder, J.
[211] L. Zhang, J.G. Han, Y.H. Guo, C.W. He, Microstructures and properties of SnZn Alloys Compd. 633 (2015) 377–383.
lead-free solder joints bearing La for electronic packaging, IEEE Trans. [240] S. Zhou, C. Yang, S. Lin, A.N. AlHazaa, O. Mokhtari, X. Liu, H. Nishikawa, Effects
Electron Devices 59 (2012) 3269–3272. of Ti addition on the microstructure, mechanical properties and electrical
[212] L. Zhang, J.-G. Han, Y.-H. Guo, C.-W. He, Properties of SnZn lead free solders resistivity of eutectic Sn58Bi alloy, Mater. Sci. Eng., A 744 (2019) 560–569.
bearing rare earth Y, Sci. Technol. Weld. Join. 17 (5) (2012) 424–428. [241] J. Shen, Y. Pu, H. Yin, D. Luo, J. Chen, Effects of minor Cu and Zn additions on
[213] Y.-H. Hu, S.-B. Xue, H. Wang, H. Ye, Z.-X. Xiao, L.-l. Gao, Effects of rare earth the thermal, microstructure and tensile properties of Sn–Bi-based solder
element Nd on the solderability and microstructure of Sn–Zn lead-free solder, alloys, J. Alloys Compd. 614 (2014) 63–70.
J. Mater. Sci.-Mater. Electron. 22 (5) (2011) 481–487. [242] F. Yang, L. Zhang, Z.Q. Liu, S.J. Zhong, J. Ma, L. Bao, Effects of CuZnAl
[214] A.A. El-Daly, A.E. Hammad, G.S. Al-Ganainy, A.A. Ibrahiem, Design of lead-free particles on properties and microstructure of Sn-58Bi solder, Materials 10
candidate alloys for low-temperature soldering applications based on the (2017) 558.
hypoeutectic Sn–6.5Zn alloy, Mater. Des. 56 (2014) 594–603. [243] Y. Li, Y.C. Chan, Effect of silver (Ag) nanoparticle size on the microstructure
[215] M.A. Wadud, M.A. Gafur, M.R. Qadir, M.O. Rahman, Effect of bismuth addition and mechanical properties of Sn58Bi-Ag composite solders, J. Alloys Compd.
on structure and mechanical properties of Tin-9Zinc soldering alloy, Mater. 645 (2015) 566–576.
Sci. Appl. 6 (2015) 792–798. [244] L. Yang, T. Li, C. Liu, S. Quan, Strengthening effect of molybdenum (Mo)
[216] Y.T. Wang, C.J. Ho, H.L. Tsai, Effect of In Addition on Wetting Properties of Sn- addition in Sn-58Bi alloy during isothermal aging, Mater. Res. Express 6
Zn-In/Cu Soldering, Mater. Trans. 51 (10) (2010) 1735–1740. (2019) 116547.
[217] A.A. El-Daly, R.E. Hammad, Effects of small addition of Ag and/or Cu on the [245] Y. Li, K. Luo, A.B. Lim, Z. Chen, F. Wu, Y.C. Chan, Improving the mechanical
microstructure and properties of Sn–9Zn lead-free solders, Mater. Sci. Eng., A performance of Sn57.6Bi0.4Ag solder joints on Au/Ni/Cu pads during aging
527 (2010) 5212–5219. and electromigration through the addition of tungsten (W) nanoparticle
[218] M. Grobelny, N. Sobczak, Effect of pH of sulfate solution on electrochemical reinforcement, Mater. Sci. Eng., A 669 (2016) 291–303.
behavior of Pb-Free solder candidates of SnZn and SnZnCu systems, J. Mater. [246] Y. Liu, H. Zhang, F.L. Sun, Solderability of SnBi-nano Cu solder pastes and
Eng. Perform. 21 (5) (2012) 614–619. microstructure of the solder joints, J. Mater. Sci.-Mater. Electron. 27 (2016)
[219] A. Basaty, A.M. Deghady, E.A. Eid, Influence of small addition of antimony (Sb) 2235–2241.
on thermal behavior, microstructural and tensile properties of Sn-9.0Zn-0.5Al [247] Y. Liu, B. Ren, M. Zhou, X. Zeng, F. Sun, Microstructure, mechanical, and
Pb-Free solder alloy, Mater. Sci. Eng., A 701 (2017) 245–253. thermal behaviors of SnBi/Cu solder joint enhanced by porous Cu, J. Mater.
[220] T. Luo, A. Hu, J. Hu, M. Li, D. Mao, Microstructure and mechanical properties Sci.-Mater. Electron. 31 (2020) 8258–8267.
of Sn-Zn-Bi-Cr lead-free solder, Microelectron. Reliab. 52 (3) (2012) 585–588. [248] N. Wu, S. Ismathullakhan, Y.C. Chan, Effect of 1wt% ZnO nanoparticles
[221] T. Gancarz, P. Bobrowski, J. Pstruś, S. Pawlak, Thermal and mechanical addition on the microstructure, IMC development, and mechanical properties
properties of lead-free SnZn-xNa casting alloys, and interfacial chemistry on of high Bi content Sn–57.6Bi–0.4Ag solder on Ni metalized Cu pads, J. Mater.
Cu substrates during the soldering process, J. Alloys Compd. 679 (2016) 442– Sci.-Mater. Electron. 25 (2014) 2169–2176.
453. [249] Z. Zhu, Y.C. Chan, F. Wu, Effects of ZrO2 nanoparticles on the mechanical
[222] J. Liu, G. Zhang, J. Ma, K. Suganuma, Ti addition to enhance corrosion properties of Sn42Bi58 solder joint, 2015 16th International Conference on
resistance of Sn-Zn solder alloy by tailoring microstructure, J. Alloys Compd. Electronic Packaging Technology (ICEPT), 2015.
679 (2015) 442–453. [250] L. Yang, J. Dai, Y. Zhang, Y. Jing, J. Ge, H. Liu, Influence of BaTiO3 nanoparticle
[223] K.I. Chen, C.H. Cheng, S. Wu, Y.L. Jiang, T.C. Cheng, Effects of Ga addition on addition on microstructure and mechanical properties of Sn-58Bi solder, J.
the wetting properties and tensile properties of Sn-Zn-Ag solder alloys, Electron. Mater. 44 (2015) 2473–2478.
Indian J. Eng. Mat. Sci. 21 (2014) 621–627. [251] C.W. Lee, Y.S. Shin, S.H. Yoo, Effect of SiC nanoparticles dispersion on the
[224] M. Ahmed, T. Fouzder, A. Sharif, A.K. Gain, Y.C. Chan, Influence of Ag micro- microstructure and mechanical properties of electroplated Sn-Bi solder alloy,
particle additions on the microstructure, hardness and tensile properties of J. Nano Res. 11 (2010) 113–118.
Sn–9Zn binary eutectic solder alloy, Microelectron. Reliab. 50 (8) (2010) [252] Y. Ma, X. Li, L. Yang, W. Zhou, M. Wang, W. Zhu, P. Wu, Effects of graphene
1134–1141. nanosheets addition on microstructure and mechanical properties of SnBi
[225] I. Shafiq, Y.C. Chan, N.B. Wong, W.K.C. Yung, Influence of small Sb solder alloys during solid-state aging, Mater. Sci. Eng., A 696 (2017) 437–444.
nanoparticles additions on the microstructure, hardness and tensile [253] X. Li, Y. Ma, W. Zhou, P. Wu, Effects of nanoscale Cu6Sn5 particles addition on
properties of Sn–9Zn binary eutectic solder alloy, J. Mater. Sci.-Mater. microstructure and properties of SnBi solder alloys, Mater. Sci. Eng., A 684
Electron. 23 (7) (2012) 1427–1434. (2016) 328–334.
[226] T. Fouzder, A.K. Gain, Y.C. Chan, A. Sharif, W.K.C. Yung, Effect of nano Al2O3 [254] X. Qiu, Q. Wang, T. Lin, P. He, F. Lu, Effect of Al18B4O33 whiskers on
additions on the microstructure, hardness and shear strength of eutectic Sn– microstructure evolution of intermetallic compound layer and shear
9Zn solder on Au/Ni metallized Cu pads, Microelectron. Reliab. 50 (12) (2010) behavior of soldered joint, Trans. Chin. Weld. Inst. 36 (2015) 35–38.
2051–2058. [255] K. Deng, Investigation on the fabrication and mechanical properties of Sn-Bi/
[227] D. Min, Ultrasonic semi-solid soldering 6061 aluminum alloys joint with Sn- Carbon Nanotubes composite, Southeast University, 2016.
9Zn solder reinforced with nano/nano+micron Al2O3 particles, Ultrason. [256] S. Zhang, Q. Chen, Fabrication of MWCNT incorporated Sn–Bi composite,
Sonochem. 52 (2019) 150–156. Compos. Pt. B-Eng. 58 (2014) 275–278.
[228] A. Sharma, A.K. Srivastava, B. Ahn, Microstructure, mechanical properties, and [257] L. Zhang, K.N. Tu, L. Sun, Y. Guo, C. He, Reviews on latest advances in
drop reliability of CeO2 reinforced Sn–9Zn composite for low temperature micro/nano-sized particles enhanced composite solders, J. Central South
soldering, Mater. Res. Express 6 (2019) 1–12. Univ. 46 (2015) 49–65.
[229] Y. Wan, S. Li, X. Hu, Y.u. Qiu, T. Xu, Y. Li, X. Jiang, Shear strength and fracture [258] K. Xu, L. Zhang, L. Gao, N. Jiang, S. Zhong, Review of microstructure and
surface analysis of Sn58Bi/Cu solder joints under a wide range of strain rates, properties of low temperature lead-free solder in electronic packaging, Sci.
Microelectron. Reliab. 86 (2018) 27–37. Technol. Adv. Mater. 21 (2020) 689–711.
57
[259] Satyanarayan, K.N. Prabhu, Wetting behaviour and interfacial microstructure [288] M. Aamir, M. Tolouei-Rad, I.U. Din, K. Giasin, A. Vafadar, Performance of
of Sn–Ag–Zn solder alloys on nickel coated aluminium substrates, Mater. Sci. SAC305 and SAC305-0.4La lead-free electronic solders at high temperature,
Technol. 27 (2011) 1157–1162. Solder. Surf. Mt. Technol. 31 (2019) 250–260.
[260] S.F. Wang, T. Yang, S.C. Lee, Wettability of electrode metals on barium [289] Z. Xia, Z. Chen, Y. Shi, N. Mu, N. Sun, Effect of rare earth element additions on
titanate substrate, J. Mater. Sci. 36 (2001) 825–829. the microstructure and mechanical properties of tin-silver-bismuth solder, J.
[261] L. Sun, M.H. Chen, L. Zhang, L.S. Xie, Effect of addition of CuZnAl particle on Electron. Mater. 31 (2002) 564–567.
the properties of Sn solder joint, J. Mater. Process. Technol. 278 (2019) [290] S. Mukherjee, M. Nuhi, A. Dasgupta, M. Modarres, Creep constitutive models
116507. suitable for solder alloys in electronic assemblies, J. Electron. Packag. 138
[262] R.K. Kaushik, U. Batra, J.D. Sharma, Structural, thermal and wetting (2016) 030801.
characteristics of novel low Bi-low Ag containing Sn–x.Ag–0.7Cu–1.0Bi [291] F.X. Che, W.H. Zhu, E. Poh, X.R. Zhang, X. Zhang, T.C. Chai, S. Gao, Creep
(x=0.5 to 1.5) alloys for electronic application, Met. Mater.-Int. (2020) 1–14. properties of Sn-1.0Ag-0.5Cu lead-free solder with Ni addition, J. Electron.
[263] Z. Moser, W. Ga˛sior, J. Pstruś, A. De˛bski, Wettability studies of Pb-Free Mater. 40 (2011) 344–354.
soldering materials, Int. J. Thermophys. 29 (2008) 1974–1986. [292] X. Kong, F. Sun, M. Yang, Y. Liu, Effect of Bi and Ni concentration on the creep
[264] L.K. Zang, Z.F. Yuan, H.Y. Xu, B.S Xu, Wetting process and interfacial behavior of the bulks of Cu/SAC/Cu micro solder joints, J. Mech. Eng. 53
characteristic of Sn–3.0Ag–0.5Cu on different substrates at temperatures (2017) 53–60.
ranging from 503 K to 673 K, Appl. Surf. Sci. 257 (2011) 4877–4884. [293] F. Tai, F. Guo, H. Shen, J. Liu, Creep properties of Ag nanoparticle reinforced
[265] T.T. Kyaw, P. Tunthawiroon, K. Kanlayasiri, K. Yamanaka, A. Chiba, A study on Sn-Cu composite solders, Rare Metal Mat. Eng. 6 (2010) 1005–1008.
wettability and formation of intermetallic phase between Co-Cr-Mo alloy and [294] F. Khodabakhshi, M. Zareghomsheh, G. Khatibi, Nanoindentation creep
Sn-Solder used as a potential under bump metallization for flip-chip properties of lead-free nanocomposite solders reinforced by modified
packages, Intermetallics 125 (2020) 106875. carbon nanotubes, Mater. Sci. Eng., A 797 (2020) 140203.
[266] W. Yang, Z. Yang, Y. Fu, A. Yu, Y. Zhan, Effect of graphene nanosheet addition [295] Y.D. Han, Y. Gao, S.T. Zhang, H.Y. Jing, J. Wei, L. Zhao, L.Y. Xu, Study of
on the wettability and mechanical properties of Sn-20Bi-xGNS/Cu solder mechanical properties of Ag nanoparticle-modified graphene/Sn-Ag-Cu
joints, Materials 13 (2020) 3968. solders by nanoindentation, Mater. Sci. Eng., A 761 (2019) 138051.
[267] J. Fan, H. Zhai, Z. Liu, X. Wang, Y. Li, H. Gao, J. Liu, Effect of Ni content on the [296] L. Zhang, J. Han, Y. Guo, L. Sun, Properties and microstructures of SnAgCu–xEu
microstructure formation and properties of Sn-0.7Cu-xNi solder alloys, J. alloys for concentrator silicon solar cells solder layer, Sol. Energy Mater. Sol.
Mater. Eng. Perform. 29 (2020) 4934–4943. Cells 130 (2014) 397–400.
[268] L. Zhang, J. Han, F. Liu, Y. Guo, C. He, Effect of nano-particles TiO2 on the [297] L. Zhang, J. Han, Y. Guo, L. Sun, Reliability of SnAgCu/SnAgCuCe solder joints
microstructures and properties of SnAgCu solders, Rare Metal Mat. Eng. 42 with different heights for electronic packaging, J. Mater. Sci.-Mater. Electron.
(2013) 1897–1900. 25 (2014) 4489–4494.
[269] Q. Lin, C. Ye, R. Sui, Wetting of Ni-based amorphous and crystalline alloys by [298] L. Yin, Z. Zhang, Z. Su, C. Zuo, Z. Yao, G. Wang, H. Zhang, L. Zhang, Y. Zhang,
Sn and Sn-based solders, Microelectron. Reliab. 111 (2020) 113722. Effects of Graphene Nanosheets on the Wettability and Mechanical
[270] D.H. Jung, J.P. Jung, Review of the wettability of solder with a wetting balance Properties of Sn-0.3 Ag-0.7 Cu Lead-Free Solder, J. Electron. Mater. 49
test for recent advanced microelectronic packaging, Crit. Rev. Solid State 44 (2020) 7394–7399.
(2018) 324–343. [299] C. Li, Y. Yan, T. Gao, G. Xu, The Microstructure, Thermal, and Mechanical
[271] X. Nan, S. Xue, P. Zhai, D. Luo, Effect of Pr addition on properties of Sn-0.5Ag- Properties of Sn-3.0 Ag-0.5 Cu-xSb High-Temperature Lead-Free Solder,
0.7Cu-0.5Ga lead-free solder, J. Electron. Mater. 45 (2016) 5443–5448. Materials 13 (2020) 4443.
[272] D.X. Luo, S.B. Xue, Z.Q. Li, Effects of Ga addition on microstructure and [300] A. Yakymovych, A. Slabon, P. Švec, Y. Plevachuk, L. Orovcik, O. Bajana,
properties of Sn-0.5Ag-0.7Cu solder, J. Mater. Sci.-Mater. Electron. 25 (2014) Nanocomposite SAC solders: the effect of adding CoPd nanoparticles on the
3566–3571. morphology and the shear strength of the Sn-3.0 Ag-0.5 Cu/Cu solder joints,
[273] N.M. Zaimi, M.M. Salleh, M.M.A.B. Abdullah, R. Ahmad, M. Mostapha, S. Appl. Nanosci. (2020).
Yoriya, D. Harvey, M., Effect of kaolin geopolymer ceramic addition on the [301] L. Zhang, N. Jiang, P. He, S.J. Zhong, Properties and microstructure evolution of
properties of Sn-3.0Ag-0.5Cu solder joint, Mater. Today Commun. 25 (2020) Sn–Cu–Ni/Cu joints bearing carbon nanotubes and graphene nanosheets for
101469. solar cell, J. Mater. Sci.-Mater. Electron. 31 (2020) 21758–21766.
[274] S. Chellvarajoo, M.Z. Abdullah, Investigation on nano-reinforced solder paste [302] M.M. Billah, Q. Chen, Strength of MWCNT-reinforced 70Sn-30Bi solder alloys,
after reflow soldering part 1: Effects of nano-reinforced solder paste on J. Electron. Mater. 45 (2015) 98–103.
melting, hardness, spreading rate, and wetting quality, Microelectron. Reliab. [303] M.Y. Xiong, L. Zhang, P. He, W.M. Long, Stress analysis and structural
84 (2018) 230–237. optimization of 3-D IC package based on the Taguchi method, Solder. Surf.
[275] S. Tikale, K.N. Prabhu, Development of low-silver content SAC0307 solder Mt. Technol. 32 (2019) 42–47.
alloy with Al2O3 nanoparticles, Mater. Sci. Eng., A 787 (2020) 139439. [304] X. Li, Z. Wang, Thermo-fatigue life evaluation of SnAgCu solder joints in flip
[276] S. Jayesh, J. Elias, Experimental investigation on the effect of Ag addition on chip assemblies, J. Mater. Process. Technol. 183 (2007) 6–12.
ternary lead free solder alloy Sn–0.5Cu–3Bi, Met. Mater.-Int. 26 (2019) 107– [305] H.H. Lee, J.B. Kwak, Realistic creep characterization for Sn3.0Ag0.5Cu solder
114. joints in flip chip BGA package, J. Electron. Mater. 48 (2019) 6857–6865.
[277] X. Hu, Y. Lai, X. Jiang, Y. Li, Effects of In addition on the wettability, interfacial [306] H. Ye, S. Xue, Z. Liang, J. Feng, Reliability evaluation of CSP soldered joints
characterization and properties of ternary Sn–Cu–Ni solders, J. Mater. Sci.- based on FEM and Taguchi method, Comput. Mater. Sci. 48 (2010) 509–512.
Mater. Electron. 29 (2018) 18840–18851. [307] H. Jeong, K.D. Min, C.J. Lee, J.H. Kim, S.B. Jung, Mechanical reliability of Cu
[278] M.L. Li, L. Zhang, N. Jiang, L. Zhang, S.J. Zhong, Materials modification of the cored solder ball in flip chip package under thermal shock test,
lead-free solders incorporated with micro/nano-sized particles: A review, Microelectron. Reliab. 112 (2020) 113918.
Mater. Des. 197 (2020) 109224. [308] L. Zhang, Z.Q. Liu, F. Yang, S.J. Zhong, Cu/SnAgCu/Cu TLP with different
[279] A.A. El-Daly, A.E. Hammad, G.A. Al-Ganainy, A.A. Ibrahiem, Enhancing thicknesses for 3D IC, Solder. Surf. Mt. Technol. 29 (2017) 151–155.
mechanical response of hypoeutectic Sn–6.5Zn solder alloy using Ni and Sb [309] L. Zhang, J.H. Cui, J.G. Han, C.W. He, Y.H. Guo, J.M. Yuan, Finite element
additions, Mater. Des. 52 (2013) 966–973. analysis of SnAgCu(Zn Co, Fe) lead-free solder joints for electronic packaging,
[280] A.A. El-Daly, A.A. Ibrahiem, M.A. Abdo, N. Eid, Viscoplastic characterization Int. J. Nonlinear Sci. Numer. Simul. 15 (2014) 197–206.
and mechanical strength of novel Sn–1.7Ag–0.7Cu lead-free solder alloys [310] L. Zhang, J.G. Han, Y.H. Guo, L. Sun, Creep behavior of SnAgCu solders
with microalloying of Te and Co, J. Mater. Sci.-Mater. Electron. 30 (2019) containing nano-Al particles, J. Mater. Sci.-Mater. Electron. 26 (2015) 3615–
12937–12949. 3620.
[281] E. Wernicki, Z. Gu, Effect of Sn nanoparticle additions on thermal properties [311] L. Zhang, L. Sun, L. Han, Y.H. Guo, Dorn creep model and finite element
of Sn-Ag-Cu lead-free solder paste, Thermochim. Acta 690 (2020) 178642. simulation of SnAgCu-CNT solder joints in FCBGA device, Int. J. Nonlinear Sci.
[282] C. Yu, Y. Yang, P. Li, J. Chen, L. Hao, Suppression of Cu3Sn and Kirkendall voids Numer. Simul. 15 (2014) 329–335.
at Cu/Sn-3.5Ag solder joints by adding a small amount of Ge, J. Mater. Sci.- [312] R.A. Athamneh, S. Hamasha, Fatigue behavior of SAC-Bi and SAC305 solder
Mater. Electron. 23 (2012) 56–60. joints with aging, IEEE Trans. Compon. Pack. Manuf. Technol. 10 (2020) 611–
[283] L. Zhang, W. Long, P. He, Y. Guo, L. Sun, N. Jiang, Effect of Ti nanoparticles on 620.
the microstructure and properties of Sn interconnect materials for 3D [313] Q.B. Tao, L. Benabou, V.N. Le, N.A.T. Nguyen, N.X. Hung, Temperature-
packaging, Rare Metal Mat. Eng. 49 (2020) 4336–4340. dependent fatigue modelling of a novel Ni, Bi and Sb containing Sn8Ag7Cu
[284] S. Liu, S. Mcdonald, K. Sweatman, K. Nogita, The effects of precipitation lead-free solder alloy, Fatigue Fract. Eng. Mater. Struct. 43 (2020) 2883–2891.
strengthening and solid solution strengthening on strain rate sensitivity of [314] S.A. Belyakov, R.J. Coyle, B. Arfaei, J.W. Xian, C.M. Gourlay, Microstructure and
lead-free solders: Review, Microelectron. Reliab. 84 (2018) 170–180. damage evolution during thermal cycling of Sn-Ag-Cu solders containing
[285] A. Yakymovych, A. Slabon, P. Vec, Y. Plevachuk, O. Bajana, Nanocomposite antimony, J. Electron. Mater. 50 (2020) 825–841.
SAC solders: the effect of adding CoPd nanoparticles on the morphology and [315] L. Zhang, L. Sun, Y.H. Guo, C.W. He, Reliability of lead-free solder joints in CSP
the shear strength of the Sn–3.0Ag–0.5Cu/Cu solder joints, Appl. Nanosci. 10 device under thermal cycling, J. Mater. Sci.-Mater. Electron. 25 (2014) 1209–
(2020). 1213.
[286] Y. Tang, Influence of nano-modifided solder on interfacial reaction and [316] B.Z. Hong, Thermal fatigue analysis of a CBGA package with lead-free solder
mechanical property of lead-free solder joints, South China University of fillets, Conference on thermal & thermomechanical phenomena in electronic
Technology, 2013. systems, 1998.
[287] E.A. Eid, A.N. Fouda, E.S.M. Duraia, Effect of adding 0.5 wt% ZnO nanoparticles, [317] L. Zhang, J.G. Han, Y.H. Guo, C.W. He, Effect of rare earth Ce on the fatigue life
temperature and strain rate on tensile properties of Sn-5.0 wt% Sb-0.5 wt% Cu of SnAgCu solder joints in WLCSP device using FEM and experiments, Mater.
(SSC505) lead free solder alloy, Mater. Sci. Eng., A 657 (2016) 104–114. Sci. Eng., A 597 (2014) 219–224.
58
[318] L. Zhang, J.G. Han, Y.H. Guo, C.W. He, Anand constitutive relation of SnAgCu- [333] Y.H. Ko, K. Son, G. Kim, Y.B. Park, D.Y. Yu, J. Bang, T.S. Kim, Effects of graphene
nano Al and the reliability of solder joints, J. Univ. Electron. Sci. Technol. oxide on the electromigration lifetime of lead-free solder joints, J. Mater. Sci.-
China 44 (2015) 471–474. Mater. Electron. 30 (2019) 2334–2341.
[319] Y.N. Wen, X.C. Zhao, Z. Chen, Y. Gu, Y. Wang, Z.W. Chen, X.Y. Wang, Reliability [334] J. Kim, K.H. Jung, J.H. Kim, C.J. Lee, S.B. Jung, Electromigration behaviors of
enhancement of Sn-1.0Ag-0.5Cu nano-composite solders by adding multiple Sn58%Bi solder containing Ag-coated MWCNTs with OSP surface finished
sizes of TiO2 nanoparticles, J. Alloys Compd. 696 (2017) 799–807. PCB, J. Alloys Compd. 775 (2019) 581–588.
[320] S. Tikale, K.N. Prabhu, Performance and reliability of Al2O3 nanoparticles [335] K.D. Min, C.J. Lee, H.J. Park, S.B. Jung, Microstructures and mechanical
doped multicomponent Sn-3.0Ag-0.5Cu-Ni-Ge solder alloy, Microelectron. properties of Sn-58wt.% Bi solder with Ag-decorated multiwalled carbon
Reliab. 113 (2020) 113933. nanotubes under 85°C/85% relative humidity environmental conditions, J.
[321] B.G. Park, W.R. Myung, C.J. Lee, S.B. Jung, Mechanical, electrical, and thermal Electron. Mater. 49 (2019) 1527–1533.
reliability of Sn-58wt.%Bi solder joints with Ag-decorated MWCNT for LED [336] L. Zhang, L. Sun, J.G. Han, Y.H. Guo, Sizes effect of CeSn3 on the whiskers
package component during aging treatment, Compos. Pt. B-Eng. 182 (2020) growth of SnAgCuCe solder joints in electronic packaging, J. Mater. Sci.-
107617. Mater. Electron. 26 (2015) 6194–6197.
[322] M.L. Li, L. Gao, L. Zhang, W. Long, S. Zhong, L. Zhang, Interfacial evolution of [337] L. Zhang, Y. Fan, S.J. Zhong, Whisker growth on SnAgCu–xPr solders in
pure Sn solder bearing silicon carbide nanowires under isothermal aging and electronic packaging, J. Mater. Sci.-Mater. Electron. 27 (2016) 5618–5621.
thermal cycling, J. Mater. Res. Technol 15 (2021) 3974–3982. [338] L. Zhang, Y. Fan, S.J. Zhong, Effect of Nd on whiskers growth behavior of
[323] J. Mehrmashhadi, Y. Tang, X. Zhao, Z. Xu, J.J. Pan, Q.V. Le, F. Bobaru, The effect SnAgCu solders in electronic packaging, J. Mater. Sci.-Mater. Electron. 27
of solder joint microstructure on the drop test failure—a peridynamic (2016) 9584–9588.
analysis, IEEE Trans. Compon. Pack. Manuf. Technol. 9 (2018) 58–71. [339] C.F. Li, Z.Q. Liu, P.J. Shang, J.K. Shang, In situ investigation on the oxidation
[324] J. Gu, Y. Lei, J. Lin, H. Fu, Z. Wu, A novel conditional probability density behavior of a RESn(3) film by transmission electron microscopy, Scr. Mater.
distribution surface for the analysis of the drop life of solder joints under 65 (2011) 1049–1052.
board level drop impact, J. Electron. Mater. 45 (2016) 145–153. [340] K.S. Kim, J.H. Kim, S.W. Han, The effect of postbake treatment on whisker
[325] S.S. Ha, J. Park, S.B. Jung, Effect of Pd addition in ENIG surface finish on drop growth under high temperature and humidity conditions on tin-plated Cu
reliability of Sn-Ag-Cu solder joint, Mater. Trans. 52 (2011) 1553–1559. substrates, Mater. Lett. 62 (2008) 1867–1870.
[326] J.Y. Park, Y.M. Kim, Y.H. Kim, Improved drop reliability of Sn-Ag-Cu solder [341] H. Hao, G.C. Xu, Y.L. Song, Y.W. Shi, F. Guo, A model for rapid tin whisker
joints by Zn addition to a Cu wetting layer, J. Mater. Sci.-Mater. Electron. 26, growth on the surface of ErSn3 phase, J. Electron. Mater. 41 (2012) 184–189.
5852-5862. [342] H. Ye, S. Xue, J. Luo, Y. Li, Properties and interfacial microstructure of Sn Zn Ga
[327] M.L. Wu, J.S. Lan, Reliability and failure analysis of SAC 105 and SAC 1205N solder joint with rare earth Pr addition, Mater. Des. 46 (2013) 816–823.
lead-free solder alloys during drop test events, Microelectron. Reliab. 80 [343] H. Ye, S. Xue, M. Pecht, Effects of thermal cycling on rare earth (Pr)-induced
(2018) 213–222. Sn whisker/hillock growth, Mater. Lett. 98 (2013) 78–81.
[328] A. Tong, Q. Fei, J. Li, Mechanical behavior of solder joints under dynamic four- [344] C.C. Jain, C.L. Chen, H.J. Lai, T.H. Chuang, The inhibition of tin whiskers on the
point impact bending, Microelectron. Reliab. 51 (2011) 1011–1019. surface of Sn-8Zn-3Bi-0.5Ce solders, J. Mater. Eng. Perform. 20 (2011) 1043–
[329] C.J. Lee, B.U. Hwang, K.D. Min, J.H. Kim, S.B. Jung, Bending reliability of Ni– 1048.
MWCNT composite solder with a differential structure, Microelectron. Reliab. [345] P. Xue, S.B. Xue, Y.F. Shen, L. Fei, H. Zhu, Mechanism of reaction between Nd
113 (2020) 113934. and Ga in Sn-Zn-0.5Ga-xNd solder, J. Electron. Mater. 43 (2014) 3404–3410.
[330] Y.H. Ko, D.Y. Yu, J. Son, J. Bang, T.S. Kim, Improving joint reliability of lead-free [346] T.H. Chuang, H.F. Wu, Effects of Ce addition on the microstructure and
solder on flexible substrate under cyclic bending by adding graphene oxide mechanical properties of Sn-58Bi solder joints, J. Electron. Mater. 40 (2011)
powder, J. Microelectron. Packaging Soc. 26 (2019) 43–49. 71–77.
[331] M. Li, J. Han, F. Guo, L. Ma, W. Zhou, Electromigration behavior of low-silver [347] G. Zeng, S. Xue, L. Gao, Z. Liang, Y. Hu, Z. Lai, Interfacial microstructure and
Sn-0.3Ag-0.7Cu-1.6Bi-0.2In solder joints, J. Electron. Mater. 49 (2020) 4237– properties of Sn–0.7Cu–0.05Ni/Cu solder joint with rare earth Nd addition, J.
4248. Alloys Compd. 509 (2011) 7152–7161.
[332] Y. Wang, J. Han, L. Ma, Y. Zuo, F. Guo, Electromigration behaviors of Cu
reinforced Sn-3.5Ag composite solder joints, J. Electron. Mater. 45 (2016)
6095–6101.
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Materials & Design 215 (2022) 110439

Contents lists available at ScienceDirect

Materials & Design

Development of lead-free interconnection materials in electronic

The effect of different element or Sn-Cu-Ni-0.5CNTs-0.05GNSs/Cu interface.

1. Introduction Agency, Waste Electrical and Electronic Equipment (WEEE) pieces

Fig. 2. Typical interface reaction model.

reaction microstructure images, the interface phase is almost all of

respond to the polymorphic transformation of Cu6Sn5, and may be

0.7Cu-xIn/Cu after reflow soldering. With the addition of 1.0 wt%

Fig. 20. Microstructures of Sn-1.0Ag-0.5Cu-xFe solder [144].

Fig. 25. Microstructures of Sn-xAg solders [178].

decrease the size of primary Zn phase significantly and refine the

Fig. 33. Sn-Bi phase diagram [230].

Fig. 35. Elemental maps of Sn-Bi-Cu solder [247].

Fig. 37. Parameters of wettability for calculation.

free solders. SAT5100 solderability test is frequently used to deter-

found that the different value of Ga content can be obtained. The

similar promotion effect in Sn-3.5Ag [172], Sn-0.7Cu [199] and

Sn0.3Ag0.7Cu Al2O3 nano 0.01–0.5 [275]

(continued on next page)

Fig. 45. The mechanism for dislocation multiplication [286].

can enhance the tensile properties of the composite solder. In the

into Sn-Ag-Cu solder, the creep strain can be decreased signifi- Dx n

0.7Cu. The low-cycle fatigue testing of series of lead-free solders

Fig. 53. Creep strain of lead-free solder joints array [315].

6.5. Reliability of solder joints under relative humidity environment

Humidity is an important index, which can affect the reliability

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