Temperature Regimes and

Chemistry for Stabilizing

Precipitation Hardening Phases
Rajesh Jha in Al–Sc Alloys: Combined
CALPHAD–Deep Machine
Department of Mechanical and Materials
Engineering; MAIDROC Laboratory,
Florida International University,

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10555 West Flagler Street,
Miami, FL 33174
e-mail: rjha001@fiu.edu
Learning
In this work, CALPHAD-based calculations provided with data for various stable and meta-
George S. Dulikravich1 stable phases in 2XXX, 6XXX, and 7XXX classes of aluminum-based alloys. These data
Fellow ASME were scaled and then used to develop Deep Learning Artificial Neural Network (DLANN)
Department of Mechanical and models for all these phases as a function of composition and temperature. Code was
Materials Engineering, written in the PYTHON programming language using TensorFlow/Keras libraries. DLANN
MAIDROC Laboratory, models were used for determining the amount of various phases for new compositions
Florida International University, and temperatures. The resulting data were further analyzed through the concept of Self-
10555 West Flagler Street, organizing Maps (SOM) and a few candidates were chosen for studying the precipitation
Miami, FL 33174 kinetics of Al3Sc phase under the framework of CALPHAD approach. This work reports
e-mail: dulikrav@fiu.edu on heat-treatment simulation for one case of 6XXX alloy where the nucleation site was
on dislocation, while a detailed study for other alloys is reported in a previously published
work. Grain-growth simulations presented in this work are valid for single crystals only.
[DOI: 10.1115/1.4054368]

Keywords: advanced materials and processing simulation, CALculation of PHase

Diagram (CALPHAD) approach, face centered cubic (FCC), Kampmann–Wagner
Numerical (KWN) approach, artificial intelligence/machine learning, data-driven design,
design of engineered materials system, innovative material synthesis and manufacturing
methods, metallic materials, microstructure property relationships

1 Introduction • 7XXX: Supersaturated solid solution transforms to GP-zones

which further transforms into η′ which finally transforms to
Aluminum is one of the most abundant elements in the Earth’s
stable η (Mg2Zn) phase. This class of alloys achieves superior
crust and has the potential of replacing steel and titanium alloys
strength when η′ and η are predominant while maximum hard-
in the automotive and aerospace sector due to its superior
ness is achieved when η′ is predominant [1].
strength-to-weight ratio [1]. One of the challenges is to develop alu-
minum alloys than possess superior mechanical properties and
are corrosion resistant at elevated temperatures of about 400 °C.
Aluminum alloy series 2XXX is Al-Cu based, 6XXX is Al-Mg-Si In aluminum-based alloys, all the metastable as well as the stable
based, while 7XXX is Al-Mg-Zn based [1]. Initial classifications phases can be present in the microstructure [2,3]. However, in ther-
of 2XXX, 6XXX, and 7XXX were based on a particular alloying modynamic calculations, one may not observe any trace of metasta-
element as mentioned below [1]. However, these alloys can ble phases in the presence of a stable phase [3].
contain several alloying elements. The precipitation sequence of Scandium (Sc) improves mechanical strength and corrosion resis-
critical phases in these alloys is as follows: tance of aluminum alloys, and the Al3Sc phase is thermodynamically
stable [1,4–6]. However, scandium is expensive and it can form a
stable Al3Sc phase up to a saturation limit [1]. Thus, scandium can
be added up to a certain amount, while the above-mentioned meta-
• 2XXX: Supersaturated solid solution transforms to GP-zones stable phases still are beneficial for achieving superior mechanical
which further transforms into θ′′ followed by θ′ which properties in these alloys. Aluminum alloys with scandium addition
finally transforms into a stable θ (Al2Cu) phase. This class may need two-step aging as Al3Sc precipitates during aging at tem-
of alloys achieves superior strength when θ′′ and θ′ are pre- peratures between 300 °C and 450 °C, while other metastable phases
dominant [1]. precipitate around 200 °C [1]. Research shows [5] that Al3Sc disper-
• 6XXX: Supersaturated solid solution transforms to GP-zones soids can be helpful in nucleation and stabilization of θ′ phase
which further transforms into β′′ followed by β′ which precipitates during aging. At the same time, an increase in copper
finally transforms to stable β (Mg2Si) phase. Here, the predom- content has a dual effect on coarsening of Al3Sc precipitates,
inant phase is β′′ , which is observed after aging [1]. as the increase in copper content can lead to both increase and
decrease of coarsening of Al3Sc precipitates [7]. Thus, it is important
1
Corresponding author.
to study the effect of composition and temperature on the stability of
Manuscript received November 19, 2021; final manuscript received April 11, 2022; stable and metastable phases in aluminum alloys with scandium
published online May 9, 2022. Assoc. Editor: Mark M. Derriso. addition.

ASME Open Journal of Engineering 2022, Vol. 1 / 011021-1

Copyright © 2022 by ASME; reuse license CC-BY 4.0
 Aluminum (Al) alloys have been studied under the framework of Table 1 Minimum and maximum concentrations for each of the
the CALPHAD approach [8–11] using Thermo-Calc software 12 alloying elements (wt%) for three series of Al–Sc-based alloys
[3,12–14]. The available literature on aluminum alloys studied (also reported in Ref. [15], reprinted with permission
through the CALPHAD approach deals with compositions of from Elsevier)
known alloys or slight deviations from known compositions [8–
2XXX Series 6XXX Series 7XXX Series
11]. Additionally, the number of elements in these alloys is rela-
tively small and varies between 3 and 8 maximum [8–11]. Element Min. Max. Min. Max. Min. Max.
Thus, the current research problem was framed so that it can
address the current limitations. In the work presented here, alloys Si 0.20 1.20 0.20 1.80 0.12 0.50
have been considered to have 12 alloying elements for 2XXX, 10 Fe 0.30 0.50 0.10 0.70 0.15 0.50
elements for 6XXX, and 11 elements for 7XXX, thus expanding Cu 3.80 6.80 0.10 0.40 0.10 2.40
the number of alloying elements of the current state of the art. Mn 0.20 1.20 0.05 1.10 0.05 0.70
Mg 0.02 1.80 0.35 1.40 0.80 3.70
Through the CALPHAD approach, one can only estimate the
Cr 0.00 0.10 0.00 0.35 0.00 0.30
stable phases. A phase associated with minimum Gibbs free Zn 0.10 0.25 0.05 0.25 3.80 8.30

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energy will be the most stable for a given composition and tempera- Ti 0.02 0.15 0.00 0.20 0.01 0.20
ture regime. Any other phase with a Gibbs free energy higher than V 0.00 0.15 0.00 0.00 0.00 0.00
that phase will be unstable or metastable, and its amount cannot be Zr 0.00 0.25 0.00 0.00 0.00 0.20
estimated through equilibrium calculations for that given composi- Sc 0.00 10.00 0.00 10.00 0.00 10.00
tion and temperature regime. In multicomponent systems like the Al Balance to Balance to Balance to
present case of aluminum alloy, there exist several metastable 100.00 100.00 100.00
phases which are important for improving multiple mechanical prop-
erties of that alloy. In order to estimate those metastable phases, one
has to suppress stable phases while performing equilibrium calcula- alloy series 2XXX, 6XXX, and 7XXX are reported in Table 1. It
tions. They must repeat these calculations multiple times in order to can be observed that in 2XXX a total of 12 alloying elements
estimate these metastable phases. Through deep learning artificial were considered. In the 7XXX series, the addition of Zr along
neural network (DLANN), a user can use the data generated with Sc was considered, while dropping V, while for the 6XXX
through the CALPHAD approach and develop the DLANN model series alloys both Zr and V were excluded. Equilibrium calculations
for each of these phases. Thereafter, they can estimate all of these were performed to stabilize the metastable phases for these alloys.
phases for thousands of new compositions in a fraction of a
second, while these calculations may take hours through the 2.1 Identification of Stable and Metastable Phases. Com-
CALPHAD approach. mercial software, Thermo-Calc 2018B [12], was used for studying
In the current work, data were generated through the CALPHAD stability of phases using the thermodynamic database TCAL5 [3]
approach [3,12–14] for various stable and metastable phases for and mobility database MOBAL4 [14]. Assadiki et al. [25] provided
2XXX, 6XXX, and 7XXX families of alloys to explore the a brief description of stabilizing metastable phases in aluminum
optimum scandium content that can be beneficial for precipitation alloys, which can be useful for studying 2XXX and 6XXX
of the Al3Sc phase along with other stable and metastable alloys. As mentioned before, in 2XXX supersaturated solid solution
phases. These data were then used to develop predictive models transforms to GP-zones which further transform into θ′′ followed by
for each of these stable and metastable phases as a function of com- θ′ which finally transforms into a stable θ (Al2Cu) phase. Thermo-
position and temperature [15]. A computer code was developed in dynamic database TCAL5 [3] and Andersen et al.’s [26] study on
the PYTHON programming language using TensorFlow [16] and various precipitates in aluminum alloys show that θ′′ closely resem-
Keras [17] libraries to develop Deep Learning Artificial Neural bles GPII zones in 2XXX, while θ-Al2Cu is the stable phase. In
Network (DLANN) models for each of the stable and metastable 6XXX, β′′ closely resembles GPII zones in 2XXX, while
phases in 2XXX, 6XXX, and 7XXX classes of aluminum alloys. β-Mg2Si is the stable phase [3,26]. For 7XXX, η-MgZn2 is the
These predictive DLANN models were then used to predict stable phase with the C14 structure, while η′ is the metastable
stable and metastable phases for new compositions and tempera- phase [27]. In the thermodynamic database TCAL5 [3],
tures. Thereafter, these data were used and analyzed through Self- V_PHASE is considered as MgZn2, while there exists another
organizing Maps (SOM) [18–20] to determine various patterns phase with C14_LAVES_PHASE in the TCAL5 database. The
within the dataset as well as for choosing a few candidate alloy structure of the GP-zones or η′ phase has been debated [26]. In
compositions to perform solidification and heat-treatment simula- the thermodynamic database TCAL5 [3], Al3Sc exists as the
tions under the framework of the CALPHAD approach. In the AL3X phase. CALPHAD approach utilizes Gibbs Energy minimi-
current work, one case of isothermal heat-treatment simulation zation as a criterion to determine the formation and stability of any
for 6XXX alloy is reported where the nucleation site is at the dis- particular phase [12,25]. In Thermo-Calc [12], it is possible not to
locations. Detailed studies of solidification and heat-treatment sim- get another metastable phase in 2XXX, 6XXX, and 7XXX,
ulations have been reported in another publication [15]. Our although it can coexist with the stable phases experimentally [3].
research group has expertise in designing alloys’ compositions
for optimal properties by the application of several concepts of arti-
ficial intelligence on data generated through experiments and data 2.2 Generation of Phase Stability Data. The prime target
generated under the framework of the CALPHAD approach phase, Al3Sc, is the stable phase. But, in aluminum alloys, superior
[18–24]. This publication is intended to provide researchers with properties are achieved by the combination of stable and metastable
a predictive tool for screening alloy compositions for phase stabi- phases. For stabilizing metastable phases, one needs to suppress the
lity prior to performing experiments. stable phases during equilibrium calculations. This way the next
phase becomes stable and its amount (volume fraction and mole
fraction) can be estimated. For example, for the 2XXX series,
1200 sets of compositions and temperature were generated and
2 Materials and Methods amounts (volume fraction) were estimated of the θ (AL2CU_C16)
In this study, 2XXX, 6XXX, and 7XXX classes of aluminum phase. For these 1200 cases, no metastable phases were observed.
alloys were chosen. These classes of alloys are heat treatable. For Therefore, the θ (AL2CU_C16) phase was removed from calcula-
each class of these alloys, variable bounds for concentrations of tion and generated 1200 sets of compositions and temperature for
alloying elements were defined based on data available in the liter- which again the amount of θ′ phase was calculated through Thermo-
ature [1,4]. These variable bounds for the chemical composition of Calc. This way, a significant amount of data was generated for

011021-2 / Vol. 1, 2022 Transactions of the ASME

stable and metastable phases for 2XXX alloys. The dataset includes 2.5 Self-Organizing Maps. Data obtained from DLANN
1200 combinations of composition and temperature for each of the models for various phases were then analyzed through the
stable and metastable phases. Similarly, a large amount of data was concept of SOM [18–20] for understanding patterns, correlations
generated for the 6XXX and 7XXX series of alloys that is suitable among variables, correlations between variables and the number
for the application of various concepts of artificial intelligence. of critical phases, and correlations among the critical phases.
SOM plots are known for preserving the topology of the dataset.
SOM maps are used to determine complex correlations in large
2.3 Data Preprocessing. Data obtained from Thermo-Calc and small datasets and are known for preserving the topology of
were not directly used. All these data were scaled. It will be men- the dataset, though the prediction capability of SOM is not accurate
tioned in the main body of the article. as each of the hexagonal units on the SOM plots are averaged
[18–20]. In this approach, accurate predictive DLANN models
were developed through the Deep Learning approach. Hence,
2.4 Deep Learning Artificial Neural Network (DLANN) SOM analysis was used for analyzing correlations and studying pat-
Template. This is a multicomponent system with multiple design terns within the dataset.

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variables. Specifically, there are 10–12 alloying elements and tem- Through SOM analysis, a set of candidate alloys was selected
perature as variables in a design process using data generated based on the optimum amount of stable and metastable phases for
through Thermo-Calc and developed predictive models for each 2XXX, 6XXX, and 7XXX alloys. SOM analysis of 6XXX alloys
of the stable and metastable phases as a function of the concentra- has been reported in the main paper, while SOM analysis of
tion of alloying elements and temperature. Computer code was 2XXX and 7XXX series alloys is reported in Appendix A.
written in the PYTHON programming language using TensorFlow
[16] and Keras [17] libraries for developing DLANN models for
2.6 Solidification and Heat-Treatment Simulations. The
each of these stable and metastable phases as a function of alloying
chemical composition of the candidate alloys was used for studying
elements and temperature for 2XXX, 6XXX, and 7XXX alloys.
the precipitation kinetics of the Al3Sc phase, where the nucleation
Prior to model development, data were scaled for all the variables
sites were in the bulk. Most of this work has been reported in
and objectives such that all values were between 0 and 1. Variables
other publications [15]. In the current work, a case for 6XXX
include composition and temperature of candidate alloys, and
series Al-based alloys is presented where isothermal heat-treatment
objectives are the amount of stable and metastable phases. There
simulations were performed at 300 °C and the nucleation sites were
were several cases for which the equilibrium amount of phase
at the dislocations. Interfacial energy between the precipitate
was 0 (zero). This is a complex dataset where too many points
(AL3X) and the matrix (FCC_L12) was optimized for this simula-
are missing. A Deep Learning Artificial Neural Network
tion. It was fixed at 0.07 J/m2. Thermo-Calc module TC-PRISMA
(DLANN) was then developed which had four hidden layers. The
uses Kampmann–Wagner Numerical (KWN) [8] approach for sim-
architecture of the DLANN is something that a user decides. For
ulating precipitation kinetics. Governing equations for KWN
example, the first hidden layer consisted of 50 neurons, and the
approach have been included in Appendix B and the companion
remaining three layers consisted of 100 neurons each. For each of
paper [15].
the alloying phases studied here, a DLANN was developed where
the initial layer was set as having 50, 60, 70, 80, 90, or 100
neurons, while each of the other three hidden layers consisted of 2.7 Computational Infrastructure
100, 120, 140, 160, 180, or 200 neurons, respectively. 2.7.1 CALPHAD-Based Work. Thermo-Calc was installed on a
This dataset was divided randomly into a training set for training desktop computer in a computer lab. The operating system was
the DLANN model and a testing set for its validation. The testing Windows 10, Core i7 processor (CPU) with 16-GB random access
set consisted of 33% of all the available data mainly to avoid over- memory (RAM). Phase transformation calculation time varied
fitting. Rectified Linear Unit (ReLU) was chosen as the activation between 20 min and 30 min, depending on the number of alloying
function, while “AdaM” was chosen as an optimizer [16,17]. elements considered for an alloy system. As mentioned, 12 elements
AdaM stands for Adaptive Moment Estimation. The stopping crite- were considered for 2XXX alloys, 10 elements for 6XXX, and 11
rion for training was the number of epochs, and it was fixed at 100 elements for 7XXX series of Al-based alloys. For heat- treatment
for all of these cases. Mean Squared Error (MSE) and Mean Abso- simulation presented in this work, it took about 3 to 4 h. In this
lute Error (MAE) over the validation set was one of the performance work, heat-treatment simulations for 6XXX alloys were performed
metrics considered for choosing a model for various stable and with 10 elements where the nucleation sites were on dislocation.
metastable phases. Tensorboard [28] was used for visualization During this simulation with the nucleation site on dislocation, the
and determining/choosing the model that can be used for predictive system crashed comparably more often than when performing simu-
tools. Apart from MAE/MSE error metrics and visualization via lations with nucleation sites in the bulk [15].
Tensorboard, the most important criterion for choosing a model
was the physical metallurgy of aluminum alloys. In this work,
2.7.2 Artificial Intelligence-Based Work. Artificial Intelligence
there are lots of missing data points for metastable phases. This
(AI)-based work was performed on a laptop. The operating system
requires giving priority to the physical metallurgy of aluminum
was Windows 10, Core i7 processor (CPU) with 32 GB RAM.
alloys. Thus, concepts of statistics and artificial intelligence are
DLANN model development took about 20–30 min depending on
used as a guiding tool, while avoiding overdependence on these
the number of alloying elements. Once the model was developed,
tools.
the prediction was done in a few seconds. DLANN models were
As mentioned, Al3Sc is a stable phase, while there are several
also used on an Android phone with 6 GB RAM and octa-core pro-
stable and metastable phases. Through the CALPHAD approach,
cessor (CPU). Prediction time was a few seconds on the Android
both stable and metastable phases cannot be estimated simulta-
phone. SOM model development took about 20–30 min for each
neously for a given composition and temperature. Separate calcula-
case.
tions need to be performed for estimating both stable and metastable
phases. Hence, DLANN models were used to estimate the amount of
stable and metastable phases for compositions and temperature in
equilibrium in case any of this information was missing. These esti- 3 Results
mates were performed for 2XXX, 6XXX, and 7XXX series alloys. 3.1 DLANN Model. Based on the literature [3,26–29] and the
Hence, a more complete dataset was created containing all the developed DLANN model, performance metrics for models for
stable and metastable phases in equilibrium for any given chemical various phases in 2XXX, 6XXX and 7XXX series alloys has
composition and temperature. been listed in Table 2.

ASME Open Journal of Engineering 2022, Vol. 1 / 011021-3

 Table 2 Performance metrics for DLANN models for various phases in 2XXX, 6XXX, and 7XXX
series of Al-based alloys

Error metrics (validation set)

DLANN Mean square Mean absolute

Alloy Phase Architecture error (MSE) error (MAE)

2XXX THETA_PRIME (θ′ ) 90-180-180-180 4.47e-4 0.01535

THETA_DPRIME (θ′′ ) 60-120-120-120 9.87e-4 0.01972
AL2CU_C16 (θ) 80-160-160-160 0.01086 0.04221
S_PHASE 50-100-100-100 4.24E-4 0.01077
AL3X (Al3Sc) 80-160-160-160 6.69e-4 0.0207
6XXX MG2SI_C1(β) 70-140-140-140 6.63e-4 0.01911
BETA_PRIME (β′ ) 80-160-160-160 8.32e-4 0.0175
BETA_DPRIME (β′′ )

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80-160-160-160 1.79e-3 0.01075
AL3X (Al3Sc) 80-160-160-160 6.09e-4 0.01898
7XXX C14_LAVES (η′ ) 50-100-100-100 6.63e-4 0.01892
T_PHASE 100-200-200-200 1.56e-3 0.01877
V_PHASE (η-MgZn2) 80-160-160-160 8.31e-3 0.04712
S_PHASE 50-100-100-100 1.76e-3 0.01604
AL3X (Al3Sc) 60-120-120-120 2.13e-5 2.9961e-3

The architecture of the DLANN model chosen in this work has temperature and concentrations of 12 alloying elements. For
been listed in Table 2. The Mean Absolute Error (MAE) in MAE at 0.04, it will be rescaled to 0.004. MAE is about 4%
Table 2 appears to be large at first glance. As mentioned in Sec. when compared with the maximum value for AL2CU_C16 (θ),
2.3, data for all the design variables and objectives were scaled which is about 0.1. Thus, although MAE and MSE appear large
between 0 and 1. DLANN models were developed for all the for a few cases, they are still between 1% and 5% of the
stable and metastable phases as a function of composition and tem- maximum value, which is still quite small for a complex problem
perature. From phase stability data, it could be observed that the like this.
maximum amount (mole fraction) of any of these phases was One can observe that the chosen model has a different structure,
numerically low (about 0.1). Mole fraction value for any of these where 50–100–100–100 represents the number of neurons in the
phases varied between 0 and 0.1. four hidden layers of the DLANN. Based on our experience,
Regarding the error metrics in Table 2, apart from AL2CU_C16 DLANN models with acceptable performance metrics MSE and
(θ), mean square errors (MSE) for all the phases are quite low, on MAE, calculated over the validation/testing set, were chosen for
the order of 1e-3 to 1e-5. AL2CU_C16 (θ) and V_PHASE further study. A reader needs to take into account that there were
(η-MgZn2) have a mean absolute error (MAE) of about 0.4. Most several cases where the amount of phase is zero, and the alloy
of the MAE values for other phases are around 0.01, while MAE system contains 9–12 alloying elements. From the data sheet,
for AL3X for 7XXX series is extremely small, of the order of 67% of data were assigned to the training set and 33% of data
1e-3. MAE of around 0.01 still seems large. However, when were assigned to the testing set, mainly to avoid overfitting.
these models will be used as a predictive tool, these results will Hence, there is a possibility to improve the performance metrics
be rescaled back to provide a practical estimate of the amount of of the models by changing these parameters.
all these phases. For example, the initial range (0–0.1) was scaled
to a new range (0–1) for model development. After these models
3.2 Self-organizing Maps Analysis. Table 3 summarizes the
are used for prediction, these data will be rescaled, or the range
error metrics of SOM analysis for 2XXX, 6XXX, and 7XXX
(0–1) will be scaled back to the range (0–0.1). Thus, even if consid-
alloys. It can be observed in Table 3, that topological error is
ering MAE at 0.01, after rescaling it will become 0.001. In a
low, while quantization error is comparatively higher. In this
complex problem with 10–12 alloying elements and a large data-
work, predictive models were developed through TensorFlow/
base with several missing values, an error of 0.001 can be accept-
Keras libraries in PYTHON [16,17] with better prediction accuracy
able, though there is still room for improvement. Again, it should
(Table 2). Thus, SOM was used for understanding patterns in the
be recalled that in this work artificial neural network (ANN)
dataset, while for prediction, the Deep Learning Artificial Neural
model with four hidden layers was developed through Deep Learn-
Network (DLANN) models were used. As mentioned before, a
ing approach. ANN models are prone to overfitting. Thus, one must
commercial software Thermo-Calc was used so that phase stability
be careful while choosing a model and using it as a predictive tool.
calculations were performed within the framework of the
As mentioned before, priority was given to physical metallurgy of
CALPHAD approach.
aluminum alloys in selecting DLANN models, while using concepts
The CALPHAD approach utilizes Gibbs Energy minimization as
of statistics and artificial intelligence for guidance. AL2CU_C16 (θ)
a criterion to determine the formation and stability of any particular
data contain lots of missing values, and there are 13 variables:
phase [12,25]. In aluminum alloys (2XXX, 6XXX, and 7XXX), tar-
geted properties are achieved by an optimum combination of stable
and metastable phases. Thermodynamically, these metastable phases
Table 3 SOM Error metrics for 2XXX, 6XXX, and 7XXX series of will be absent in the presence of stable phases, but kinetically these
Al–Sc-based alloys metastable phases have been observed in the microstructure of alu-
minum alloys [2,3]. In order to stabilize a metastable phase, one
Quantization error Topological error
needs to remove the stable phases while performing calculations
2XXX 0.126 0.030 for the stability of metastable phases. In this work, a complex multi-
6XXX 0.109 0.034 component system for 2XXX, 6XXX, and 7XXX series alloys was
7XXX 0.131 0.017 chosen. It can be possible that a certain metastable phase can be
absent for a certain composition and temperature combination

011021-4 / Vol. 1, 2022 Transactions of the ASME

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Fig. 1 SOM plot of components for alloying elements, and critical phases in 6XXX series of
Al-based alloys along with Sc and temperature

even after the stable phases are removed from the calculation as regime around 200 °C and are unstable at elevated temperatures
several other equilibriums exist in a multicomponent system. Deter- [1]. SOM maps were able to recognize this pattern and correctly posi-
mining these compositions and temperature regimes can be helpful tioned the candidate alloys on the vertices of hexagonal units in a
in screening alloys prior to performing experiments. Thus, SOM way that the predictions can be verified through concepts of physical
plots can be used to determine the composition regime prior to per- metallurgy. Even though the SOM algorithm does not operate on
forming precipitation kinetics simulations for the Al3Sc phase or principles of physical metallurgy, still it was able to mimic these
experiments. vital correlations. This proves the efficacy of the application of
SOM maps in materials design as in this problem the database con-
tains several missing points, which is quite common in materials/
3.3. 6XXX Alloys. Figure 1 shows the component plot for alloy design problems. In Fig. 2, one can additionally observe that
6XXX alloys. In Fig. 1, one can observe that elements Al, Sc, elements aluminum, scandium, and AL3X phase are correlated.
and the phase AL3X are clustered together or are correlated. This An increase in aluminum and scandium results in an increase in
relation can be established as an increase in Al and Sc will lead the AL3X phase, which can be understood as the Al3X phase, in
to an increase in AL3X (Al3Sc) phase. In Fig. 1, MG2SI_C1 (β) this case, is Al3Sc.
and BETA_PRIME (β′ ) phases are clustered together. From the One of the goals of this work is to determine the scope of working
physical metallurgy of aluminum alloys, one can establish this rela- with small concentrations of Sc since Sc is expensive. From Fig. 2,
tion as BETA_PRIME (β′ ) is a metastable phase, which finally it can be observed that it is possible to work with a lower amount
transforms into a stable MG2SI_C1 (β) phase [1]. of Sc (<wt. 2%) at lower temperatures since BETA_PRIME,
Figure 2 shows the distribution of Sc, temperature, and a few BETA_DPRIME, and MG2SI_C1 phases are stable. Heat treatment
critical phases for 6XXX series. SOM maps consist of hexagonal of aluminum alloys in the case of Sc addition is performed in two
cells. Values visible on SOM maps are the average value over a stages. The annealing temperature for precipitating BETA_PRIME,
cell. Hexagonal cells are not visible in Fig. 2 since a significantly BETA_DPRIME, and MG2SI_C1 phases is performed at around
large number of candidate alloys are included in this study; thus, 100–200 °C, while the annealing temperature for precipitating
the SOM map looks pixelated. AL3X is usually above 300 °C. Thus, SOM maps proved to be
In Fig. 2, BETA_PRIME (β′ ) and BETA_DPRIME (β”) exist in helpful in determining candidates for performing solidification
the lower temperature regime (∼180 °C) and is nonexistent at ele- and heat-treatment simulations. Based on the preceding computa-
vated temperature (540 °C). Additionally, MG2SI_C1 (β) phase tional effort, the most promising Al–Sc-based alloy from each of
exists in a larger amount in a lower temperature regime (∼180 °C). the three Al-based series (2XXX, 6XXX, and 7XXX) was selected
From the physical metallurgy of aluminum alloys, BETA_PRIME for heat-treatment simulation as reported in Table 4. Candidates
(β′ ) and BETA_DPRIME (β′′ ) are the metastable phases that reported in Table 4 are also reported in Ref. [15], where simulations
finally transform into the thermodynamically stable MG2SI_C1 were performed for solidification and heat treatment for studying
(β) phase [1]. Additionally, MG2SI_C1 (β), BETA_PRIME (β′ ), the precipitation kinetics of the Al3Sc phase for these candidate
and BETA_DPRIME (β′′ ) phases are stable in the temperature alloys [15]. These compositions were obtained from artificial

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Fig. 2 Amount of critical phases (mole) in 6XXX series of Al-based alloys along with Sc (wt%) and temperature (°C)

intelligence-based algorithms. Practically, it is not possible to grain size of the Al3Sc phase at dislocations, available literature
achieve similar compositions as shown in Table 4. [1] was consulted. Depending on the application, Al3Sc grain size
can vary from 2 to 100 nm. Strengthening in aluminum alloys is
achieved by precipitation hardening and also mechanical working.
3.3.1 Heat-Treatment Simulations. In Ref. [15], simulations In this work, dislocation density was fixed at 6.0 × 1012 m−3. The
were performed where nucleation sites for precipitation of Al3Sc mechanical treatment introduces many dislocations in the system.
phases were in the bulk. In the current work, precipitation kinetics Thus, studying the precipitation kinetics of Al3Sc crystals with dis-
simulation of the Al3Sc phase was at the nucleation site which is at locations as a nucleation site will be helpful for researchers working
the dislocations. A candidate alloy corresponding to the 6XXX on aluminum alloys. In Ref. [15], the mean radius of the crystals
series from Table 4 was used, and isothermal annealing was per- increases continuously when the nucleation sites were in the bulk.
formed at the dislocations at 300 °C. A system of 10 alloying ele- In this work, nucleation sites are at the dislocations. A detailed anal-
ments, and no reported information on interfacial energy for such ysis at other temperatures will be helpful to quantify the effect of
a complex system. In this work, the reference temperature was time on overall grain size.
chosen as 300 °C. In Ref. [15], temperatures were chosen
between 300 °C and 450 °C, where all the nucleation sites were
in the bulk. Figure 3(a) shows the variation of the mean radius of
the grain over the annealing time, which was set at 1000 h.
4 Discussion
Figure 3(b) shows the variation of volume fraction over annealing
time. From Figs. 3(a) and 3(b), it can be observed that the mean In this work, the research problem was formulated in a way
radius and volume fraction of Al3Sc crystals increase initially and which will be helpful in expanding the domain of the current
saturate at about 67 h. After 67 h, there is minimal change in the state of the art or available literature on aluminum alloys studied
growth of Al3Sc crystals. Interfacial energy was optimized by under the framework of the CALPHAD approach.
trials and in this case, it was set at 0.07 J/m2. For the optimal The novelty of this work can be summarized in a few points as
follows:
Table 4 Compositions (wt%) of three series of Al-based alloys • Literature on aluminum alloys using the CALPHAD approach
chosen for solidification and heat-treatment simulation in a usually focuses on compositions which are around the known
previously published work [15] (reprinted with permission compositions of standard alloys [25]. In this work, a frame-
from Elsevier)
work was developed to predict and test novel compositions
Alloying element 2XXX Series 6XXX Series 7XXX Series
through a thorough investigation based on the CALPHAD
and Artificial Intelligence. Novel compositions can be ana-
Si 0.38828 1.5497 0.28606 lyzed through DLANN models and the equilibrium amount
Fe 0.3919 0.57313 0.21862 of various stable and metastable phases can be estimated in
Cu 4.95088 0.27893 1.51113 2XXX, 6XXX, and 7XXX classes of aluminum alloys
Mn 0.32005 0.63697 0.36188 through this approach.
Mg 0.53321 1.07076 1.05662 • Literature on aluminum alloys using the CALPHAD approach
Cr 0.04353 0.1437 0.12353 usually focuses on alloys with 6–8 alloying elements
Zn 0.19235 0.11882 3.73898 [4–11,25–29]. In this work, 12 alloying elements were consid-
Ti 0.04297 0.13088 0.15506
V 0.09389 0.0 0.0
ered for the 2XXX alloy system, 10 alloying elements for
Zr 0.21774 0.0 0.17829 6XXX, and 11 alloying elements for 7XXX series Al-based
Sc 0.92541 2.60077 0.75953 alloys, which will be helpful for researchers to utilize the pre-
Al 91.89979 92.89525 91.61031 sented approach in their own work, providing room for the
addition of new elements in their existing alloys.

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Fig. 3 Precipitation kinetics of Al3Sc phase at dislocation for isothermal annealing at 300 °C for 6XXX series in Table 4: (a) mean
grain radius (nm) and (b) volume fraction

• Scandium is added to aluminum alloys along with zirconium metastable phases for aluminum alloys under the framework of the
[30,31] and has a profound effect on mechanical properties CALPHAD approach. CALPHAD (Thermo-Calc) databases are
in aluminum alloys. Both elements contribute to improvement created from actual experiments and atomistic simulations, while
in strength, hardness, and stress corrosion resistance. [30,31]. DLANN models were developed under the framework of Tensor-
In a previously published work [15], alloys containing Zr Flow/ Keras libraries that are known for determining nonlinear and
were considered for Scheil solidification simulation and pre- complex correlations. The presented approach provides predictive
cipitation kinetic simulation of the Al3Sc phase [15]. The DLANN models that can be used for new chemical compositions
current work is mainly focused on determining novel compo- and temperatures to determine stable and metastable phases in the
sitions for 2XXX, 6XXX, and 7XXX alloys while determining alloys at the same instant, as experimentally these phases coexist,
the scope of Sc addition. Heat-treatment simulation performed but thermodynamically stable and metastable phases cannot
in this work is for the 6XXX alloy in Table 4, which does not coexist. Thereafter, data predicted through DLANN models were
contain any zirconium. This work cannot be compared with utilized to study 2XXX, 6XXX and 7XXX series Al–Sc-based
Refs. [30,31] as Zr containing alloy was not considered for systems and the stable and metastable phases in each of these
heat-treatment simulation. A previously published work [15] systems by utilizing Self-Organizing Maps (SOMs). SOMs are
can be compared to some extent. known for determining complex correlations between design vari-
• Solidification and heat-treatment simulations were performed ables and objectives and also correlations among the objectives.
and have been reported in a previously published work [15]. Models developed through TensorFlow/Keras libraries have low
In the current work, precipitation kinetics simulation results error and SOM analysis of these alloys also shows low topological
with the nucleation site at the dislocation have been included. error. Based on this work, a few of the most promising chemical
Isothermal annealing was performed at 300 °C. For the 6XXX compositions requiring low concentrations of Sc were developed
alloy in Table 4, interfacial energy was optimized, and the for performing heat-treatment simulations.
value is 0.07 J/m2. From Fig. 3, it can be observed that the Solidification and heat-treatment simulations were performed on
grain growth occurs in the beginning till about 67 h. After candidate alloys listed in Table 4 and had been reported [15]. In the
67 h, grain size becomes stable as even up to 1000-h annealing current work, heat-treatment simulations for 6XXX alloy at 300 °C
time there is minimal change in grain size. were performed where the nucleation sites were at dislocations.
From the results, it can be observed that the average grain size
Heat-treatment simulations require optimized values of interfa-
stabilizes at about 67 h, and there is minimal change in grain size
cial energy between precipitate and the matrix phase in order to
afterward even when isothermal simulations were performed for
mimic experimental findings, which is a must from an application
1000 h. In this case, interfacial energy for the Al3Sc phase was opti-
point of view. Thus, our planned future work will focus on optimiz-
mized. The presented work forms the basis for future work on opti-
ing [20] interfacial energy at various nucleation sites for multicom-
mizing interfacial energy for various nucleation sites. Grain-growth
ponent aluminum alloys with scandium addition.
simulations presented in this work are valid for single crystals only.

5 Conclusions Acknowledgment
This study presents a novel computational approach that can be The authors would like to express their sincere gratitude to Pro-
utilized for screening candidate alloys prior to performing experi- fessor Cristian Ciobanu from the Colorado School of Mines for
ments by estimating the equilibrium amount of various stable and providing access to some of the commercial software used in this
metastable phases in aluminum alloys containing scandium. In this paper. Thanks, are also due to Professor Carlo Poloni from
work, Deep Learning Artificial Neural Network (DLANN) was ESTECO Company for approving the free use of ESTECO’s soft-
developed by utilizing a database generated for various stable and ware modeFrontier in this research.

ASME Open Journal of Engineering 2022, Vol. 1 / 011021-7

Funding Data were stabilized by suppressing the stable phases. Still, vital informa-
tion on the interaction between components, components and
• This work was supported by the College of Engineering and various phases, and interaction between different phases were
Computing at Florida International University and by NASA obtained through SOM analysis. Thus, it is possible to utilize
HQ University Leadership Initiative (ULI) program under SOM to determine the composition regime where a researcher can
federal award number NNX17AJ96A titled “Adaptive Aero- study precipitation kinetics of the Al3Sc phase.
structures for Revolutionary Supersonic Transportation” Figure 5 shows the distribution of Sc, temperature, and a few crit-
managed by Texas A&M University. ical phases for the 2XXX series. From Fig. 5, one can observe that
Sc directly affects the amount of AL3X phase at all temperatures.
Phase AL2CU_C16 is a thermodynamically stable phase, while
Conflict of Interest THETA_PRIME and THETA_DPRIME metastable phases. In
There are no conflicts of interest. This article does not include Fig. 5, THETA_PRIME, THETA_DPRIME, and AL2CU_C16
research in which human participants were involved. Informed phases are stable at lower temperatures, which is also reported in
consent is not applicable. This article does not include any research the literature [1]. In Fig. 5, it can be additionally observed that THE-

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in which animal participants were involved. TA_PRIME and THETA_DPRIME are stable to a certain extent at
moderate temperatures (above 200 °C), while AL2CU_C16 is
absent for this temperature regime. Here, 200 °C is the average tem-
Data Availability Statement perature of candidate alloys included in those SOM cells. Hexago-
nal cells are not visible since there are too many candidate alloys
Raw data set and developed models are for internal use and included in this study; thus, the SOM map looks pixelated. Any
cannot be shared with this article. region on the SOM map that is marked above 200 °C consists of
alloys for which the average temperature is above 200 °C. Heat
treatment for precipitating Al3Sc (AL3X) is performed at 300 °C
Appendix A or above, while for precipitating THETA_PRIME and THETA_D-
2XXX Alloys. Figure 4 shows the component plot for 2XXX PRIME, heat treatment is performed below 200 °C. Thus, the occur-
alloys, where all the variables (composition and temperature) and rence of a few candidate alloys with a significant amount of
the objectives (critical phases) are positioned in a way that if any THETA_PRIME and THETA_DPRIME will be helpful in design-
two or more of them are together, it means that they are correlated. ing new heat-treatment protocols for these classes of alloys. SOM
This information is beneficial for an experimentalist in understand- algorithm proved to be useful in understanding various features/cor-
ing the correlations between various design variables and objectives relations in the dataset that can be validated by concepts of physical
simultaneously. In Fig. 1 and Fig. 4, one can observe that elements metallurgy of aluminum alloys. This demonstrates the efficacy of
Al, Sc, and the phase AL3X are clustered together or are correlated. pattern recognition through SOM maps.
This relation can be established as an increase in Al and Sc will lead
to an increase in AL3X (Al3Sc) phase. In Fig. 4, THETA_PRIME
(θ′ ) and THETA_DPRIME (θ′′ ) phases are clustered together.
From the physical metallurgy of aluminum alloys, one can establish 7XXX Alloys. Figure 6 shows the component plot for 7XXX
this relation as metastable phase THETA_DPRIME (θ′′ ) transforms alloys. It can be observed from Fig. 6 that AL3X, Sc, and Al are
into another metastable phase THETA_PRIME (θ′ ), which finally adjacent to each other. Thus, SOM plots were able to detect corre-
transforms into stable AL2CU_C16 (θ) phase. It should be men- lations between the concentrations of Al, Sc, and stable phase
tioned that the SOM algorithm has no information on Gibbs AL3X. One can also observe that minor elements like Si, Zr, Mn,
energy minimization, the theory on which these databases predict Fe, Cr, and Ti are clustered together on the map. There does not
a certain phase. Still, the SOM algorithm is able to capture informa- seem to be any other strong correlations between design variables
tion shown in the literature [1]. Alloying elements such as Si, Zr, Zn, and desired phases, as C14_LAVES and V_PHASE are close, but
Mn, Fe, Cr, Ti, and V are present in small amounts and are clustered not close enough to draw any definitive conclusion. Figure 7
together on the map. The alloy system under consideration is a shows the distribution of Sc, temperature, and a few critical
complex multicomponent system, where the metastable phases phases for 7XXX series. From Fig. 7 it can be observed that Sc
directly affects the amount of AL3X phase at all temperatures.
C14_LAVES, V_PHASE and S_PHASE is stable at a lower
temperature, marked around 170 °C on the SOM map. Above
170 °C, stability decreases for these phases. Here 170 °C is the
average temperature for the candidate alloys included in the hexag-
onal units or cells. Thus, it can be possible that for a number of can-
didate alloys there can be traces of these phases and for a few
candidates these phases can be in a larger or acceptable amount
from a metallurgical point of view. This information will be
helpful in designing new chemical compositions and manufacturing
protocols for these alloys.
Figure 7 shows the distribution of Sc, temperature, and a few crit-
ical phases for the 7XXX series. From Fig. 4 it can be observed that
Sc directly affects the amount of AL3X phase at all temperatures.
C14_LAVES, V_PHASE, and S_PHASE are stable at a lower tem-
perature, marked around 170 °C on the SOM map. Above 170 °C,
stability decreases for these phases. Here, 170 °C is the average
temperature for the candidate alloys included in the hexagonal
units or cells. Thus, it can be possible that for a number of candidate
alloys, there can be traces of these phases and for a few candidates
these phases can be in a larger or acceptable amount from a metal-
Fig. 4 SOM plot of components for alloying elements, and crit- lurgical point of view. This information will be helpful in designing
ical phases in 2XXX series of Al-based alloys along with Sc and new chemical compositions and manufacturing protocols for these
temperature alloys.

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Fig. 5 Amount of critical phases in 2XXX series of Al-based alloys along with Sc and temperature

Fig. 6 SOM plot of components for alloying elements, and critical phases in 7XXX series of
Al-based alloys along with Sc and temperature

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Fig. 7 Amount of critical phases in 7XXX series of Al-based alloys along with Sc and temperature

One of the goals for this work was to explore the possibility of Sc
 
addition in small amounts (<2 wt%). Through this work, it became ∗ −ΔG∗
possible to find the compositions and temperature regimes for Js = Zβ N0 exp (B3)
kT
which Al3Sc (AL3X) and other stable and metastable phases are
stable in significant amounts. Based on the preceding computational In Eqs. (B2) and (B3), Z which stands for Zeldovich factor, β∗ is
effort, the most promising Al–Sc-based alloy from each of the three the attachment rate of solute atoms to the precipitate (AL3X), N0
Al-based series was selected for heat-treatment simulation as denotes the number of nucleation sites available in the beginning,
reported in Table 4 in the main article and also in a previously pub- ΔG∗ is the Gibbs energy of formation of a precipitate, k is Boltz-
lished work [15]. mann’s constant, and T is absolute temperature [12,13,32–38]. In
Eq. (B2), θ can vary but in Thermo-Calc it is fixed at 2 [13].
The number density of precipitates, in the beginning, can be
shown as in Eq. (B4), while the number density (Nt) at any
Appendix B instant of time (t) can be expressed as in Eq. (B5) [13]
Kampmann–Wagner Numerical Approach. TC-PRISMA  
module [13] in Thermo-Calc [12] utilizes the KWN approach for −ΔG∗
N0 exp (B4)
simulating precipitation kinetics of a precipitate which involves kT
nucleation, growth, and coarsening [32–36]. This section explained
the governing equations and lists the parameters used while simulat- 
ing precipitation kinetics.
Nt = Jt dt (B5)
In this work, the matrix is the FCC_L12 phase. The precipitate is
AL3X, which is Thermo-Calc notation for Al3Sc. The molar
volume of the precipitate was taken from the Thermo-Calc data- ΔG∗ is the Gibbs energy (or activation energy) of formation of the
base. The grain aspect ratio was fixed at 1.0, while the mobility precipitate can be expressed as in Eq. (B6). ΔGFCC−Al
m
3 Sc
is the molar
enhancement factor was fixed at 5. Gibbs energy of formation of Al3Sc nanocrystals from the FCC
An initial number of nucleation sites (N0) were calculated from matrix and VmAl3 Sc is the molar volume of Al3Sc nanocrystals [34],
dislocation density, which was fixed at 6.0 × 1012/m3. Interfacial while σ is the interfacial energy between the FCC matrix phase
energy was set at 0.07 J/m2. and precipitate Al3Sc phase
Time-dependent nucleation rate (Jt) can be derived from classical
nucleation theory [37] and is expressed as in Eq. (B1) 16π σ 3int

−τ ΔG∗ =  2 (B6)
3 ΔG FCC−Al 3 Sc
Jt = Js exp (B1) m
t VmAl3 Sc
In Eq. (B1), τ is incubation time which can be further simplified
as shown in Eq. (B2), t is the time and Js is the steady-state nucle- Zeldovich factor (Z ) and β∗ can be expressed as shown by
ation rate as shown in Eq. (B3) [37–40] Eqs. (B7) and (B8), respectively [13,39–41]

1 VmAl3 Sc σ
τ= (B2) Z= (B7)
θZ 2 β∗ 2πNA R∗2 kT

011021-10 / Vol. 1, 2022 Transactions of the ASME

 ⎡ ⎤
2 −1
∗2
2πR ⎣ (XiAl3 Sc − XiFCC ) ⎦
β∗ = (B8)
(lAl3 Sc )4 XiFCC DFCC
i

In Eq. (B8), XiFCC and XiAl3 Sc are the equilibrium composition of

element i in the FCC and in the Al3Sc phase respectively, while
DFCC
i is the chemical diffusion coefficient of element i in the FCC
phase [39–42].
For Al3Sc crystals, critical radius (R∗ ) [30–33] and time-
dependent radius (RAl t
3 Sc
) [41,42] can be expressed as in
Eqs. (B9) and (B10), respectively.

2σVmAl3 Sc
R∗ =−

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(B9)
ΔGFCC−Al
m
3 Sc

dRAl
t
3 Sc
DFCC Xi,tFCC − XiFCC Fig. 8 JMAK analysis for volume fraction estimations
= i
(B10)
dt ξi,t RAlt
3 Sc
X Al3 Sc − X FCC
i i

FCC
In Eq. (B10), Xi,t is the composition of the supersaturated FCC
matrix phase and XiAl3 Sc is the equilibrium composition of the Al3Sc
FCC
phase. The growth of Al3Sc crystals is dependent Xi,t . Thus, the
mass balance equation can be expressed as shown in Eq. (B11) [40]

FCC
Xi,t = (Xi,0
FCC
− VfAl3 Sc XiAl3 Sc )/(1 − VfAl3 Sc ) (B11)

In Eq. (B10), parameter ξi,t can be expressed as in Eq. (B12),

while parameter λi,t in Eq. (B12) can be calculated by solving
Eq. (B13) [40–42]

1 Xi,t FCC
− XiFCC
ξi,t = 1 − λi,t π exp (λ2i,t )erfc(λi,t ) = 2
(B12)
2λi,t X Al3 Sc − X FCC
i i

√ X FCC − XiFCC

2λ2i,t − 2λ3i,t πexp(λ2i,t )erfc(λi,t ) = i,t (B13) Fig. 9 JMAK analysis for estimation of the mean radius of the
XiAl3 Sc − XiFCC grain
Coarsening rate of the precipitate can be predicted from the
growth equation shown in Eq. (B14) [42–44]
JMAK equation shown in Eq. (C1) [45]
  n 
dRAl
t
3 Sc
8 σVatAl3 Sc DFCC XiFCC t
= i
(B14) fv (t) = fv0 1 − exp − (C1)
dt 27 (RAl3 Sc )2 kT XiAl3 Sc − XiFCC tr
JMAK analysis for estimating the evolution of the Al3Sc phase
In Eq. (B14), VatAl3 Sc is the mean atomic volume of the Al3Sc
has been analyzed for a better understanding of nucleation and
phase, while NA is the Avogadro’s number
growth phenomenon. Figure 8 shows the relevant plot for volume
VmAl3 Sc fraction, while Fig. 9 shows the relevant plot for the mean radius.
VatAl3 Sc = (B15) In Fig. 8, one can observe that a perfect straight line was not
NA obtained as expected. In Fig. 9, a straight line can be observed.
Time-dependent mean radius and volume fraction of Al3Sc nano- As mentioned throughout this text, this is a completely new
crystals at any time step can be calculated through Eqs. (B16) and system. It was studied under the framework of the CALPHAD
(B17), respectively [39–42] approach, where usually 3–6 elements are analyzed at a time.
Thus, some discrepancies are unavoidable. Our group is working
 on improving model development within the framework of the
N RAl3 Sc
RAl
t
3 Sc
= t t (B16) CALPHAD approach and expects to improve the models to their
Nt maturity and use toward experiments.

3
4π(RAl
t
3 Sc
)
V Al
f ,t
3 Sc
= Nt (B17) References
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011021-12 / Vol. 1, 2022 Transactions of the ASME