TAGC1 de 1
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by the
vii
An aperture in a metal film can be regarded as the complementary structure of
a wire. In Chapter 4, we address the emission of light through a rectangular
nanoaperture as an antenna problem. We demonstrate, explicitly, that resonant
nanoslot antennas display a magnetic dipole response. Such antennas offer an
efficient interface between emitters and surface plasmons.
The excitation or detection of a dipolar emitter from the far field involves
large solid angles. To address quantum emitters efficiently, a low divergence of
their radiation patterns is needed. To this end, in Chapter 5 we develop and
realize unidirectional optical antennas. We show how the emission of a quantum
emitter is directed by multi-element Yagi-Uda and log-periodic optical antennas
and demonstrate directional operation of a single-element design based on a split-
ring resonator.
Light emission usually occurs through electric dipole transitions because
multipolar emission rates are orders of magnitude slower. In some materials,
however, multipolar optical transitions do occur. In Chapter 6, we assess through
simulations the feasibility of enhancing magnetic dipole and electric quadrupole
transitions with several realistic nanoantenna designs.
The results in this Thesis demonstrate the potential of optical antennas as
elements to control light on the nanoscale, based on radio and microwave antenna
engineering. Within this powerful paradigm, the interaction of light with
nanoscale matter can be tailored with complete flexibility.
Such a degree of control over light emission and absorption may have a
practical impact in spectroscopy, sensing, display technologies, lighting,
photovoltaics, and general optical and optoelectronic devices.
viii
Resumen
x
Acknowledgments
xi
Contents
xiii
4.3. Characteristics of resonant nanoslot modes ............................ 49
4.4. Discussion and conclusions ..................................................... 51
5. Directional Nanoantennas .....................................................53
5.1. Directing light on the nanoscale ............................................. 54
5.2. Yagi-Uda nanoantennas ......................................................... 56
5.3. Log-Periodic nanoantennas..................................................... 63
5.4. Magneto-Electric nanoantennas.............................................. 73
6. Antenna-Enhanced Forbidden Transition Spectroscopies ......79
6.1. Multipolar transitions in spectroscopy ................................... 80
6.2. Enhancing forbidden transitions ............................................. 81
6.3. Magnetic dipole emission enhancement .................................. 83
6.4. Electric quadrupole emission enhancement ............................ 87
6.5. Conclusions............................................................................. 89
Conclusion .................................................................................91
Bibliography ..............................................................................93
List of Publications ................................................................. 109
xiv
1.
Optical Antennas
Molecules, ions, atoms and semiconductors are emitters of light
behind core technological applications. In general, interaction with
nanoscale materials, at the single quantum emitter level is
inefficient. Thus, one of the main tasks of modern Optics is the
development of more effective optical interfaces between light and
the nanoscale. In this Chapter, we introduce the concept of a
nanoantenna as an optical element to control light on the nanoscale
based on radio and microwave antenna engineering. We describe
the main physical mechanisms that allow antennas to control light,
explaining the basic elements of optical antenna theory. Finally, we
explore the applications that can potentially benefit from the
design paradigm of optical antennas.
1
1. Optical Antennas
2
1.1 Nanoscale light-matter interaction
field, with low divergence fields such as plane waves or Gaussian beams. More
efficient interfaces between light and nanoscale matter are thus required.
3
1. Optical Antennas
4
1.2 Controlling light with optical antennas
5
1. Optical Antennas
The opposite is also possible, and the external quantum efficiency with an
antenna may be lower than the intrinsic one, a situation known as quenching.
Due to the rapid increase in the non-radiative rate at close proximity to a metal
surface, the distance of emitter to antenna must be controlled to be within the
optimal range of 5-12 nm [6, 7].
Control of directionality
The angular radiation pattern of an object determines how easily it can be
addressed from the far field. The radiation pattern of a quantum emitter is
typically dipolar, with angular emission covering a wide range of solid angles.
Interaction with an emitter can be made more efficient by coupling it to an
antenna with an angular pattern matching the detection or illumination angles,
directing the emission or excitation into the optical system. An increase in the
collection efficiency ηc results in a higher observed intensity.
Furthermore, emission can be converted to another, well-defined
electromagnetic mode in the far field, with properties different to the original
source. Examples include the conversion of an electric dipole emitter into a
quadrupolar source or a mode in an optical fiber.
The directionality of a radiation pattern P(θ,ϕ), where θ is the inclination
angle (latitude) and ϕ is the azimuth angle (longitude) in spherical coordinates,
can be quantified by several metrics, including:
6
1.2 Controlling light with optical antennas
Directivity
Power density at a given angle compared to the total integrated power
distributed isotropically over all directions:
D(θ,ϕ)=4πP(θ,ϕ)/∫P(θ,ϕ)dΩ
An isotropic source would have a directivity of 1, a dipole has a directivity
of 1.5, and directional antennas typically achieve values of 10-25.
Gain
To take into account not only the shape of the radiation pattern but also
the radiation efficiency, the directivity is multiplied by the quantum
efficiency:
G=ηD
Front-to-Back Ratio
Power emitted in the direction of maximum emission P(θmax, ϕmax) divided
by the power radiated in the diametrically opposite direction:
F/B= 10 log(P(θmax,ϕmax)/P(θmax+π,ϕmax)),
or F/B=10 log(P(θmax,ϕmax)/P(θmax,ϕmax+π))
if the emission is contained only in one half-space.
Beam-Width at Half-Maximum
Angular width of the main radiation lobe.
Polarization control
An optical antenna can control the polarization of the interaction, both in the far
and near fields. In the far field, the antenna mode can determine the emission or
excitation polarization [11, 12]. In the near field, it can convert an external
polarization into another local polarization of the evanescent fields. This local
conversion between polarizations also enables their use as nanoscale interfaces
between freely-propagating and guided waves of a specific polarization (e. g.,
surface plasmons or waveguide modes). In- and out-couplers to such modes can be
devised, with control of the local phase distribution.
7
1. Optical Antennas
Spectral control
Excitation or emission through a resonant antenna can shape the wavelength
spectrum of the interaction [13]. This interaction usually occurs in the weak-
coupling regime and the spectral response of the coupled emitter-antenna system
is given by the product of the individual spectral responses of emitter and
antenna [14]. In contrast, if the interaction strength reaches the strong-coupling
regime, emitter and antenna cannot be separated as independent entities and the
linear relation of spectral enhancement breaks down.
8
1.3 Fundamentals of optical antennas
times shorter than the vacuum wavelength. The slope of the linear scaling of the
resonances with length depends on material (metal dispersion and surrounding
medium) and geometrical (width and height) parameters [16, 17]. For an Au
nanowire of 55 nm of width and 37 nm of height surrounded by air, the spectrum
of emission of a dipolar emitter coupled to the nanoantenna is presented in Fig.
1.3c. For example, a 150-nm long antenna is resonant around a wavelength of 700
nm. In our experiments, antennas will be lying on a glass substrate, resulting in
an additional shortening of the resonant lengths, around 1.5 times less.
The angular radiation pattern of such an antenna is very similar to a point
electric dipole oriented along the long axis of the nanowire (Fig. 1.3b), which
draws a parallel with the resemblance of a radio-frequency λ/2 dipole antenna to
a point Hertz electric dipole [3]. The angular pattern contains then two lobes with
9
1. Optical Antennas
a sin(θ)2 angular dependence and rotational symmetry around the axis of the
dipole.
The electric field is concentrated at the ends of the nanowire. At resonance, an
emitter excites the antenna mode efficiently from one side of the antenna; both
ends light up with comparable strength (Fig. 1.3e). Off resonance, however, the
emitter couples inefficiently to the antenna mode; the original point dipole
dominates the field distribution with a maximum at the source position (Fig.
1.3f).
The half-wave electric dipole antenna is a basic building block for other
antenna designs. For example, two laterally shifted antennas can form a resonant
gap antenna, further increasing the local field enhancement. An array of detuned
dipole antennas is the basis for multi-element directional antennas, such as the
popular Yagi-Uda design used in television reception. Finally, the understanding
of the fundamental resonance of a nanowire is necessary to investigate higher
order resonances in nanowires, with contributions to the emission from other
multipoles. It proves also helpful in understanding the fundamental magnetic
resonance of a nanoslot antenna, the complementary structure of a nanowire.
Consequently, the λ/2 dipole antenna will prominently feature as the starting
point of the discussion of all the Chapters in this Thesis.
10
1.4 Potential applications
Spectroscopy
Due to their broad spectral response, metal nanoantennas are particularly
suitable for room-temperature single-molecule studies. In the tradition of
metal-enhanced spectroscopies, they can improve fluorescence, Raman,
infrared vibrational and non-linear spectroscopies.
Single-Photon Sources
Photons are quantum information carriers and nanophotonic devices could
offer a route for scalable quantum information technologies. By enhancing
transition rates and directing the emission into specific electromagnetic
modes, antennas can increase the maximum repetition rate and brightness
of single photon sources [19].
Near-Field Optics
Field localization can contribute towards optimized scanning near-field
microscopy probes for nanometer-resolution imaging and spectroscopy [10].
Furthermore, the antennas can be tailored to interact with specific
polarizations of the electric and magnetic fields.
Photodetectors and Photovoltaics
Light-harvesting and emission devices based on thin films can be improved
through the integration of optical antennas. For example, local field
enhancement can focus the incident field to weakly-absorbing materials
such as thin-film photovoltaics or graphene. In a photodetector, reducing
the active material volume [20] allows for faster speeds thanks to improved
carrier collection. Electro-optical devices in general can employ metallic
antennas also as electrodes, combining electrical and optical functionalities
[21].
Nonlinear Optics
In nonlinear optical processes, the signal scales at least quadratically with
the local field. Resonant antennas, especially gap antennas, are
particularly suited due to their field enhancement [22]. The non-linear
response of external materials can be improved. The metal itself has a
strong nonlinear susceptibility, resulting in two-photon luminescence, and
second or third harmonic generation. They might be used as localized
sources of coherent radiation.
Other Nanophotonic Components
Photonic and plasmonic circuitry can benefit from the interfacing to free-
space radiation offered by antennas. A network of optical antennas might
be more efficient for nanoscale point-to-point links than plasmonic
11
1. Optical Antennas
12
2.
Experimental Methods
for Nanoantennas
We introduce the experimental methods used in this Thesis for the
characterization of light emission by optical nanoantennas. Firstly,
we describe a technique to attach quantum dots to nanoantennas
at predefined positions, a very flexible approach to couple light
sources in the near field. The resulting emitter-antenna systems are
characterized by confocal photoluminescence microscopy with
polarization resolution, which allows a first quantification of the
coupling of emitter and antenna. Importantly, we describe the
angular measurement technique of back focal plane imaging for
recording angular radiation patterns of nanoscale objects. In
combination, these experimental methods are a powerful tool for
the study of any nanoantenna design, regardless of the nature of its
electromagnetic mode.
13
2. Experimental Methods for Nanoantennas
14
2.2 Coupling an emitter to a nanoantenna
15
2. Experimental Methods for Nanoantennas
coating. This polymer is functionalized; an amino group caps the QD surface. The
total QD diameter is expected to be below 15 nm. The QD emission is centered
around 790 nm with a full width at half maximum of 80 nm. Such long
wavelengths are attainable thanks to the use of the alloyed ternary compound
CdSeTe instead of the more usual CdSe core.
For the two lithographic steps, we employ polymethyl methacrylate (PMMA)
as a positive electronic resist, spun-cast onto a glass substrate with a 10-nm layer
of indium tin oxide (ITO). The first e-beam lithography defines the Au antennas
and alignment markers, formed by thermal evaporation of a 30-40 nm Au layer
and subsequent lift-off. The markers are used as a reference to accurately overlap
the second lithographic layer, which sets the boundaries for the formation of a
self-assembled monolayer of mercapto-undecanoic acid (MUA).
Specificity to gold is provided by the thiol groups of MUA, which physically
adsorb on the Au surface. Next, a carbodiimide (EDC) activates the carboxylic
acid terminations of MUA, so that the amino groups of the QDs can bind to them
covalently. Finally, once the QDs are deposited and immobilized, the remaining
PMMA is lifted off by rinsing in acetone with the sample in vertical orientation to
avoid sticking of undesired QDs. The process flow is summarized in Figure 2.1. As
a final result, we attain an accuracy of around 40 nm in positioning a QD patch
relative to a metal structure, given by the resolution of the lithography.
To conclude, this fabrication technique will allow us to position a few emitters
at designated positions on an arbitrary metal nanostructure. Using close to ideal
16
2.3 Imaging a nanoantenna
point sources, this method is a very powerful tool for the study of optical
nanoantennas.
17
2. Experimental Methods for Nanoantennas
basis for angular detection. The sample is excited by a circularly polarized He-Ne
laser beam (λ=633 nm), with a power of a few µW after reflection on a long-pass
dichroic mirror. The laser is focused to the diffraction limit in order to address
one antenna at a time. The resulting luminescence is separated from the
excitation wavelength with a long-pass filter. For alignment of the optical system,
we use small clusters of quantum dots or dye-loaded fluorescent nanospheres.
Polarization analysis
The confocal signal is split by a polarizing beam-splitter cube onto two detection
channels with avalanche photodiodes (Perkin Elmer, SPCM-AQR-14 and 16). The
18
2.3 Imaging a nanoantenna
confocal aperture size is given by the area of the detectors. The two polarization
channels enable polarization-resolved imaging; by calculating the degree of linear
polarization DOLP=(I║-I⊥)/(I║+I⊥), we represent the polarization anisotropy of
the emission, where I║ is the counts detected in the vertical polarization (parallel
to the long axis of a linear antenna). The DOLP is one of the Stokes parameters
that parameterize the polarization of light.
The images can be color-coded for degree of linear polarization, with
brightness for each pixel proportional to the number of counts. Red (green) color
represents vertical (horizontal) linear polarization, whereas yellow may be
unpolarized emission or any polarization with a 45° degree projection on the
image plane. The two APD signals are calibrated to account for differences in the
quantum efficiencies of both detectors and for polarization by the optical elements
(e. g., induced by the dichroic mirror upon oblique reflection/transmission).
Coupling of an emitter to an antenna can lead to a complete modification of
the polarization. The change in polarization (color) is evident in Figures 2.3, 2.4
19
2. Experimental Methods for Nanoantennas
and 2.5. These images are conclusive proof of the ability of our double lithography
technique to attach emitters to the antennas deterministically.
On the other hand, for a quantitative comparison of simulations with
experimental polarization measurements, the calculated emitted fields must be
also propagated through the confocal imaging system using the angular spectrum
representation [31] [32]. The use of a high numerical aperture objective (non-
paraxial imaging) for a linearly polarized nanoscale source (dipole) results in
additional polarization components in the image plane. As a consequence, the
highest value of DOLP that can be measured with our system is 0.9, even for a
linearly polarized point source with nominal DOLP=1.
20
2.3 Imaging a nanoantenna
along the scanning direction (e.g., in Figures 3.2 and 5.1). The non-radiative
mechanisms that have been suggested to produce intermittency in emission [33]
are based on the ionization of the QD or the existence of surface trap states. In
our experiments, several factors might influence blinking simultaneously: the
metal nanoparticle [35, 36]; the ITO substrate [37]; excitation power, rapid aging
21
2. Experimental Methods for Nanoantennas
under ambient conditions, and functionalization involving thiol groups [38] and
solvents.
Photon anti-bunching measurements directly reveal non-classical light emission
by the antennas. By using a non-polarizing beam-splitter instead of a polarizing
cube, we turn our microscope into a Hanbury Brown and Twiss set-up to record
the correlated arrival times of pairs of photons. The dip in photon coincidences
around zero inter-photon delay time (Fig. 2.7a) is characteristic of single photon
emission [39-41], confirming that as few as a single quantum dot can be attached
to an antenna.
For N perfect single-photon emitters, the normalized coincidence rate at zero
delay follows the dependence 1 - 1/N. As seen in the case of a QD without
antenna, our QDs are not ideal single-photon sources because bi-excitons provide
a non-negligible probability of emitting two photons simultaneously. Furthermore,
luminescence of the antennas themselves also contributes background photons.
The finite temporal resolution around zero delay also increases the observed
coincidences above zero.
22
2.4 Measuring the angular radiation pattern of a nanoantenna
Yet, the coincidences remain under 0.5, demonstrating that most photons
come from a single quantum emitter. For a better contrast in single-photon
emission, other emitters with lower bi-exciton rates or other antenna materials
with lower autoluminescence might be used. Other examples of antennas with
photons arising mostly from 2, 3 and 4 QDs are shown in Fig. 2.7b. In all cases,
coupling to the antenna increases transition rates (radiative, non-radiative and
excitation rates) resulting in a narrower dip than for a single QD on bare glass
(black line).
To conclude, we find thanks to these photon-counting measurements that the
number of QDs coupled to each antenna is usually between 1 and 3, with a most
frequent value of 2 or 3, when the combination of two steps of lithography and
chemical functionalization is used.
23
2. Experimental Methods for Nanoantennas
The coordinates and power density of the emission as recorded on the BFP are
related to the angular radiation pattern (power density per unit solid angle) by a
projection given by the design of the microscope objective [46]. To assess the
particular relation followed by our objective, we used several diffraction gratings
to calibrate the k-space images with the known angles of the diffraction grating
orders. We found that our objective satisfies the sine condition [46], that is to say,
the coordinates on a BFP image (radius R) are related to the inclination angle (θ)
between the optical axis and the wave vector by the relation R(pixel)=K sinθ,
where K is a calibration constant related to the magnification of the imaging
system. The intensity on the back focal plane of the objective (k-space) is related
to the angular pattern by I(θ,ϕ)=IBFP(kx, ky) cos(θ), where kx=K R sin(θ) cos(ϕ)
and ky=K R sin(θ) sin(ϕ). The cosine factor is an apodization factor introduced
for conservation of energy, to account for the different solid angles covered by the
area of a pixel at different BFP positions. When comparing our experimental
results to simulations, we discard the last few pixels of the BFP image because
transmission goes down gradually near the numerical aperture.
24
2.4 Measuring the angular radiation pattern of a nanoantenna
The radiation patterns as obtained in the BFP for a single molecule (DNQDI)
in a thin PMMA film and a single QD embedded in a thin PMMA film are shown
in Fig. 2.8. In all k-space images, we observe two distinct circles: the maximum
collection angle of our objective (θNA=72.8°) and the critical angle of a glass-air
interface (θcrit=41.1°). Most of the radiation is emitted towards the substrate and
it is contained between the critical angle and the numerical aperture angle. In the
case of a single molecule (Fig. 2.8a), the anisotropic pattern of a single electric
dipole with two lobes can be clearly identified [42].
Our QDs exhibit a degenerate transition dipole moment oriented almost
isotropically on a “bright” plane [47-51], originating in the crystalline structure
and shape of the semiconductor nanocrystals. As a result, the radiation pattern of
even a single QD is nearly isotropic in the azimuthal angle ϕ, and its emission is
approximately unpolarized (Fig. 2.5). We find only minor differences between the
patterns of different QDs, and their emission can be described by a superposition
of in-plane electric dipoles. This observation is confirmed when a linear polarizer
is used to analyze the QD angular pattern (insets in Fig. 2.8b); the patterns then
resemble two single, linear electric dipoles, as for the single molecule case.
Finally, to understand intuitively why the radiation pattern of a dipolar source
peaks at the critical angle, we note that the fields of a point source contain
evanescent components. Emission at angles beyond the critical angle arises from
these fields [52]. Snell’s law must be used to propagate the fields of a dipole from
air into the dielectric; a plane wave is refracted at the critical angle for an
incidence angle of 90°, and higher angles of refraction can only be obtained with
imaginary angles out of the plane-wave angular spectrum. By bringing the source
close to a dielectric interface, the evanescent fields can be funneled to the far field.
This situation is reciprocal to the excitation of evanescent fields under total
internal reflection.
25
3.
Nanowire Antennas for
Multipolar Radiation
We demonstrate controlled emission of a quantum emitter into
multipolar radiation through selective coupling to a linear nanowire
antenna. In general, multipolar transitions other than electric
dipoles are too weak to be observed at optical frequencies in single
emitters such as fluorescent molecules and quantum dots, because
they have dimensions much smaller than the wavelength of light.
Therefore, they emit predominantly as point electric dipoles. In this
Chapter, an antenna resonance tailors the interaction of a quantum
dot with light, effectively creating a hybrid nanoscale source
beyond the simple Hertz dipole. Our findings establish a basis for
the controlled driving of fundamental modes in nanoantennas and
metamaterials, for the understanding of the coupling of quantum
emitters to nanophotonic devices such as waveguides and
nanolasers, and for the development of innovative quantum nano-
optics components.
27
3. Nanowire Antennas for Multipolar Radiation
28
3.2 Resonant nanowires as optical antennas
29
3. Nanowire Antennas for Multipolar Radiation
In other words, plasmons travel along the antenna (length L) with complex wave
vector k and are reflected at the antenna ends with complex reflection coefficient
r=|r|eiφ. The plasmon propagating along the antenna has a wavelength λSP
(Re(k)=2π/λSP) and losses determined by Im(k)=ki.
Resonances are found at lengths that satisfy the condition Ln = λSP/2 (n-φ/π),
where n is a positive integer. These parameters are retrieved by fitting to
experimental results in polarization and angular measurements. This model
describes the emission of the antenna mode alone, regardless of the number of
emitters coupled to it, and does not include possible contributions of emission
that is not coupled to the antenna mode. Note that the presence of the
semiconductor nanocrystals will slightly perturb the antenna parameters.
The emission properties of these modes and their near-field interaction with
quantum emitters are governed by the symmetry and spatial distribution of the
characteristic currents for each mode. For example, the lowest order mode, j=1,
has odd charge symmetry (Figure 3.1a) and its current distribution creates a
dipole source. The j=2 mode has even symmetry, with a zero net dipole moment,
and resembles a longitudinal quadrupole. Hence, j=1 corresponds to a half-wave
dipole antenna, whereas j=2 is a full-wave, end-fed quadrupole antenna. As a first
approximation, we expect that the angular radiation patterns of these two lowest
order antenna modes are point dipoles and point quadrupoles (Figures 3.1c and d
for an antenna on a glass substrate and Figure 3.1e for free space).
30
3.2 Resonant nanowires as optical antennas
31
3. Nanowire Antennas for Multipolar Radiation
32
3.3 Multipolar radiation of a quantum dot
After taking into account this partial coupling of QDs to the antenna mode,
our one-dimensional cavity model reproduces the observed oscillations in average
polarization with a fit (Figure 3.3b, blue line) based on a superposition of the
theoretical antenna emission plus an incoherent sum of two perpendicular
polarizations describing uncoupled emission. The antenna parameters retrieved by
fitting to the average polarization are presented in Table 3.1.
The average polarization decreases for increasing order of modes because the
resonances are damped due to dissipation, resulting in a lower coupling efficiency.
This average represents the inhomogeneously broadened distribution of antennas
in the arrays, similarly to the broadened spectrum of an ensemble of molecules.
Individual antennas exhibiting higher degrees of polarization are singled out from
this ensemble (squares in Figure 3.3b). We focus next on these individual cases,
where the emitter-antenna coupling is stronger.
33
3. Nanowire Antennas for Multipolar Radiation
34
3.3 Multipolar radiation of a quantum dot
The j=2 resonance has even charge symmetry and its radiation pattern is
oriented perpendicular to the first mode (Figure 3.4d), corresponding to a linear
or longitudinal quadrupole. Due to their opposite symmetry, the central
horizontal maximum in the emission of the dipole becomes a minimum in the
emission of the quadrupole, despite their equally parallel polarization along the
antenna. This is a clear illustration of the non-equivalence of polarization and
angular measurements; in general, the observation of a polarization cannot be
attributed to a single antenna mode with a characteristic angular pattern.
The third order resonance has the symmetry of the half-wave dipole antenna
but its lobes are now narrower (Figure 3.4e), a characteristic of higher multipoles.
For increasing order modes additional lobes appear, with alternating symmetry
and positions of minima and maxima. Related patterns have been measured
recently in the electroluminescence, cathodoluminescence and far-field scattering
of antennas of different resonant orders [21, 65, 74] and in the emission of
photonic crystal cavities [75]. The sharp features of our patterns gradually wash
out for higher order resonances due to a lower coupling, which results in a
rotationally symmetric background added to the pure antenna modes. For longer
wires [55, 57, 71], several resonances start overlapping within the luminescence
spectrum of the QD, and a band pass filter was used to select the central part of
the emission spectrum for j=5 and j=6 to improve the contrast (Figures 3.4g-h).
The j=2 resonance illustrates the physics involved. This antenna efficiently
converts the emission of a dipolar transition (QD) into quadrupolar radiation by
coupling to the optical antenna. Its angular pattern consists of two broad lobes
directed along the antenna and resembles the pattern of a point quadrupole on
glass (Figure 3.1d). The coupling of a dipole transition to a quadrupolar mode is
possible because the placement of the QD at the end of the antenna breaks the
inversion symmetry of the QD-antenna system. Because the total antenna length
(260 nm) is on the order of half the wavelength, the j=2 mode radiates effectively
[70]. It is therefore neither sub-radiant nor dark, despite its even charge
symmetry. For antennas, multipolar moments are not necessarily small and, for
antenna dimensions on the order of the wavelength, the radiant character of the
mode is independent of its multipolar nature.
Multipolar and dipolar antenna modes radiate with a comparable rate, in
contrast to multipolar transitions in small quantum emitters such as molecules,
quantum dots or ions, which are usually several orders of magnitude slower in
radiative rates than dipolar transitions. Indeed, the ratios of average detected
luminescence per antenna for the different modes are Ij=1: Ij=2: Ij=3: Ij=4 = 1: 0.4:
0.25: 0.3, with oscillations in radiated power following those of the polarization
response in Figure 3.3b. In absolute terms, the average count rate for the dipolar
35
3. Nanowire Antennas for Multipolar Radiation
resonance (Ij=1) is 135 kCounts per ms for an excitation power density of 1.08 kW
cm2. A QD coupled to the j=2 mode thus provides a novel nanoscale system: a
bright single quantum emitter that interacts with light as a quadrupole.
.
From this current distribution, we obtain the emitted field as:
,
where kx and ky are the projections of the wave vector (of magnitude k0) of the
emitted radiation along the in-plane x and y coordinates, and E0(kx, ky) is the
electric field emitted by a y-oriented electric dipole above an air-glass interface
[76]. This dipole is situated 15 nm away from the interface on the air side, at half
the experimental antenna height of 30 nm.
The radiation pattern of each individual antenna was reproduced using a least-
squares linear fit to find the optimal weights of the antenna mode and the
uncoupled background for different sets of antenna parameters (see Section 3.1 for
definitions). We found the best fit to the individual antennas for the values of
antenna parameters summarized in Table 3.2. The parameters related to the
losses and the reflectivity of these individual antennas have a better quality than
the inhomogeneously broadened average antenna obtained from polarization
measurements in Table 3.1.
36
3.3 Multipolar radiation of a quantum dot
37
3. Nanowire Antennas for Multipolar Radiation
modes. For higher order resonances, even modes are composed of a coherent
superposition of predominantly even multipoles; complementarily, odd modes are
dominated by odd multipoles. This expansion also demonstrates that the
background contribution (green bars in Figure 3.5) increases and starts
dominating for higher order modes as expected for a decreasing coupling
efficiency.
39
3. Nanowire Antennas for Multipolar Radiation
40
3.4 Other signatures of antenna resonances
41
3. Nanowire Antennas for Multipolar Radiation
42
4.
Nanoslot Antennas at
Magnetic Resonance
In this Chapter, we address the emission of light through a
nanoaperture in a metal film as an antenna problem. We
demonstrate, explicitly, that resonant nanoslots display a
predominantly magnetic dipole response. We observe clear
differences in the angular radiation patterns of resonant and non-
resonant antennas, and compare our results to calculations with
magnetic and electric dipole sources, respectively. At resonance,
angular radiation patterns evidence the dominant magnetic dipole
character, accompanied by a more efficient launching of surface
plasmons. Off resonance, angular patterns are divergent beams, as
for electric dipoles. The resonant magnetic mode is preserved even
when plasmons are suppressed by a chromium layer. Through
simulations, we draw a parallel with an electric dipole nanowire
antenna, in agreement with Babinet's principle. Our results
highlight the potential of resonant nanoslot antennas as interfaces
between photons, emitters, and propagating surface plasmons.
43
4. Nanoslot Antennas at Magnetic Resonance
44
4.2 Probing nanoslot modes
45
4. Nanoslot Antennas at Magnetic Resonance
46
4.2 Probing nanoslot modes
antenna were not present. The situation is thus similar to the inefficient coupling
to non-resonant nanowires seen in the previous Chapter. The results are therefore
consistent with two perpendicular electric dipoles of QDs close to a mirror (Fig.
4.4c), not coupled to any antenna mode. The angular patterns are in agreement
with recent results on non-resonant apertures as the basis of more complex
antenna designs [18, 113], and are qualitatively similar to diffraction through
near-field aperture probes [133, 134].
At resonance, the angular pattern is strikingly different due to efficient
coupling of the emitters to the antenna mode, now dominating in Fig. 4.3b. The
emission is linearly polarized across the slot, with a 7:1 intensity ratio between
perpendicular polarizations (Fig. 4.2b). With the two lobes characteristic of
47
4. Nanoslot Antennas at Magnetic Resonance
48
4.3 Characteristics of resonant nanoslot modes
49
4. Nanoslot Antennas at Magnetic Resonance
mode is clearly beyond cut-off, with a small effective refractive index of 0.02 and
high losses on the order of 100 dB/µm. No sharp variations of waveguide
propagation constants were observed around the resonance and, hence, we discard
the waveguide resonance found for larger apertures at the lowest order mode cut-
off [137, 140].
On the other hand, vertical Fabry-Pérot cavity resonances require thicker
metal films [135] and they are roughly independent of the perimeter. They can
thus be disregarded as the origin of our resonances. Note that, for thicker films,
Babinet's principle will eventually break down even qualitatively due to the
appearance of vertical modes.
50
4.4 Discussion and conclusions
51
4. Nanoslot Antennas at Magnetic Resonance
52
5.
Directional
Nanoantennas
Nanoscale quantum emitters are key elements in quantum optics
and constitute the ultimate limit in sensing. However, efficient
optical excitation and detection of such emitters involves large solid
angles because their interaction with freely-propagating light is
omnidirectional. In this Chapter, we present unidirectional
antennas for controlling the emission of single quantum emitters.
By coupling quantum dots to the near field of an antenna, the
emission is determined by the antenna mode in polarization and
radiation pattern. We demonstrate experimentally the operation of
a Yagi-Uda antenna driven by a single emitter. Next, we explore
through simulations the optimization of such multi-element
antennas with a log-periodic design. Finally, we show both with
experiments and theory that a single split-ring resonator is a
particularly suitable directional design that harnesses the
interference of magnetic and electric components. These results
open new possibilities for effective communication of light to, from
and between nano-emitters.
53
5. Directional Nanoantennas
54
5.1 Directing light on the nanoscale
55
5. Directional Nanoantennas
56
5.2 Yagi-Uda nanoantennas
57
5. Directional Nanoantennas
58
5.2 Yagi-Uda nanoantennas
to 0.5 (Fig. 5.3, left) because the QDs have different orientations and the gold
squares induce no preferential direction. The corresponding angular emission
pattern is shown in Fig. 5.4a. All ensuing momentum-space images contain two
distinct circles in the polar angle θ: the outer circle is the maximum collection
angle of our objective (θNA=72.8°), while the inner circle is the critical angle for
the glass-air interface (θc=41.1°). A dipole close to an interface emits primarily
into the high index medium, with sharply peaked maxima at the critical angle.
Moreover, our QDs exhibit a degenerate transition dipole moment contained on a
“bright” plane [47, 48]. As a result, the radiation pattern of a QD is nearly
isotropic in the azimuthal angle ϕ.
When coupled to a λ/2 dipole resonant nanoantenna (Fig. 5.3, center), the
picture changes dramatically: the QD luminescence turns into a clear linear
polarization parallel to the long axis of the antenna (DOLP ≈ 0.8) and the
radiation pattern transforms to that of a linear dipole close to an interface [42].
These are two clear signatures of the near-field coupling [11]. Remarkably, the QD
emission becomes fully determined by the antenna mode, both in polarization and
direction, despite the degeneracy of the QD dipole moment.
59
5. Directional Nanoantennas
60
5.2 Yagi-Uda nanoantennas
61
5. Directional Nanoantennas
62
5.3 Log-Periodic nanoantennas
Although hardly any directed emission is observed for the complete spectrum
(Fig. 5.6, top row), a high directivity is recovered when only the long wavelength
part of the spectrum is selected (Fig. 5.6, second row from the bottom). For short
wavelengths, below a cut-off value, the emission is even reversed with the main
lobe pointing backwards, a fact also present in our numerical simulations. We
observe a similar behavior for the longer antenna YU160, with all characteristic
wavelengths shifted to longer wavelengths. For shorter antennas, YU110 and
YU125, the antennas are blue-detuned with respect to the quantum dot spectrum
and a lower directivity is observed for the full spectrum.
In summary, by tuning the antenna or selecting certain emission bands, we
have proved the frequency dependence of the directivity of an optical Yagi-Uda
antenna.
Conclusions
We have demonstrated the unidirectional emission of quantum-dot–Yagi-Uda
systems; the antenna transforms the non-directional quantum-dot luminescence
into a directed light source which can now be efficiently collected with lower
numerical aperture optics. By reciprocity, we anticipate that the antennas work
both in emission and absorption. Most remarkably, all this control over photon
emission is obtained from an antenna that is only a single wavelength long.
Further optimization of the many Yagi-Uda design parameters, including the
addition of more director elements, might sharpen up the unidirectional cone.
This trend will eventually saturate when metal losses start to dominate the multi-
element scattering. The operation bandwidth can be increased through the use of
a Log-Periodic design [3], which we study in the next Section. An inherent
problem of the Yagi-Uda design for optical frequencies is the need to position the
source to drive locally one individual element, which might not be compatible
with some of the potential applications. We will explore in the next Sections
designs that alleviate this requirement.
63
5. Directional Nanoantennas
between the lengths, separations and widths of the elements. Moreover, the source
can be located at the end of different antenna elements, distributing the role of
the feed element. We systematically study the influence of geometrical parameters
on angular performance and local field enhancement to find optimum values.
Next, we demonstrate that introducing a gap in the dipole array architecture can
provide at least a ten-fold enhancement of the emitted power. Finally we present
an optical zigzag antenna capable of both broader spectral response and even
higher directivity.
64
5.3 Log-Periodic nanoantennas
recent simulations [183, 184] for antenna designs based on tapered dipole arrays
revealed directional and multiband characteristics. In the present study, we report
on the performance of strictly self-similar LP antennas, accounting for the effects
of the different parameters.
Three flavors of LP antennas will be studied based on arrays of different unit
elements: dipole nanowire antennas, gap antennas, and nanowires connected in
zigzag. The geometrical parameters defining a dipole-array LP antenna are
illustrated in Fig. 5.7a. The scaling factor r (or its reciprocal value τ) is the ratio
between the lengths (an and an+1) of two consecutive elements, as well as between
two consecutive widths (bn and bn+1) and between inter-element distances (dn and
dn+1): r=1/τ=an/an+1=bn/bn+1=dn/dn+1. Hence, only one of the element lengths an
suffices to define all the other lengths, once the scaling factor r is fixed. The
distance dn between adjacent elements with numbers n and n+1 can be expressed
normalized to the element length [3], thus defining an inter-element distance
factor: σ=dn/2an. The parameters τ and σ are also related to the antenna apex
half angle by α=tan-1(1-τ)/4σ. The geometrical description of the antenna is
completed with the definition of the aspect ratio of the elements AR = an/bn, the
element thickness and the edge rounding. The number of elements (N), the length
of one given element (an), the scaling factor (r) and the inter-element distance (σ)
were systematically varied for dipole-array antennas in order to investigate their
effect on the directivity, local field enhancement and radiated power.
Although analytical methods can be applied for the study of relatively simple
multi-element nanoantenna architectures [172, 174, 185, 186], we will employ the
Finite-Difference Time-Domain (FDTD) method because it is an approach
suitable for our complex three-dimensional objects. All FDTD simulations were
65
5. Directional Nanoantennas
66
5.3 Log-Periodic nanoantennas
For sufficiently small inter-element distance (σ) or scaling factor (r) the field
enhancement is expected to occur simultaneously at different elements because
adjacent resonances have overlapping bandwidths. At resonance, the field
enhancement for forward illumination is generally an order of magnitude smaller,
except at the longest element n=1, which is similar to the reflector in a Yagi-Uda
antenna. Away from the resonance, the forward intensity can be similar or even
higher than the backward intensity at particular wavelengths. Therefore, by
reciprocity, bi-directionality or even backward directivity should be expected in
emission configuration for a source at that position.
67
5. Directional Nanoantennas
68
5.3 Log-Periodic nanoantennas
69
5. Directional Nanoantennas
5.10) and even in a lateral direction rather than in forward direction (not shown).
Backward emission was already demonstrated experimentally for detuned Yagi-
Uda antennas in Section 5.2, while lateral emission can be associated with the
asymmetric position of the source with respect to the antenna axis (y).
70
5.3 Log-Periodic nanoantennas
71
5. Directional Nanoantennas
Conclusions
We have presented systematic simulations of several types of log-periodic optical
antennas. The dipole array design was investigated in detail with focus on
72
5.4 Magneto-Electric nanoantennas
73
5. Directional Nanoantennas
robust against changes in the position of the local source, bringing directional
optical antennas closer to practical applications.
Magneto-electric interference
A magneto-electric antenna exploits the interference between magnetic and
electric modes as a principle of operation. The fields radiated by alternating
electric and magnetic multipoles have opposite symmetries, which can be used for
the design of optical antennas with a target radiation pattern. The interference of
both a magnetic dipole (MD) and an electric quadrupole (EQ) with an electric
dipole (ED) can lead to directional radiation. The concept of magneto-electric
interference is schematically explained in Fig. 5.14c for a MD perpendicular to an
ED. For an antenna, if both dipoles are excited simultaneously, the emission can
be directed to the forward or backward directions depending on the relative phase
between both dipoles.
For implementation of this principle at optical frequencies, nanostructures
with coexisting multipolar resonances are required. The directional scattering of
dielectric nanospheres supporting magnetic dipole Mie resonances has been
demonstrated recently both theoretically and experimentally [99, 165, 188-191].
Other particles that exhibit directionality as a result of multipolar interference are
metal-dielectric nanoshells and nanocups [166, 192].
Specifically, we will employ a split-ring resonator architecture (SRR), known
for its optical magnetic response. The resonances of SRRs have been studied
extensively within the context of metamaterials [96, 193-195]. A U-shaped SRR
design with a carefully chosen geometry (Fig. 5.14a) allows us to optimize the
directionality through the balance between different multipolar components.
Similarly to a gap antenna, the width and the separation between the SRR arms
can be used for improving the coupling of ED emitters to the antenna mode
thanks to local electric field enhancement. The two arms are connected by a
bridge, whose width controls how much the antenna differs from two parallel,
unconnected wires.
74
5.4 Magneto-Electric nanoantennas
75
5. Directional Nanoantennas
76
5.4 Magneto-Electric nanoantennas
two factors are responsible for the robustness of the directionality for broadband
emitters randomly attached to the antennas. Importantly, the external quantum
efficiency of the emitter-antenna system remains over 70% within the bandwidth
of the QD as required for a good antenna design.
Angular radiation patterns are also obtained in simulations, confirming the
experimentally observed directional emission with F/B ratios over 10 dB for
wavelengths between 750 and 850 nm for a dipole inside the gap. When the dipole
is at the top end of the gap, the antenna emits in the opposite direction but the
radiated power is much lower for all wavelengths within the bandwidth of the QD
(gray lines in Fig. 5.16b). The net result is that the SRR antenna emits
directionally even for emitters randomly positioned on the antenna.
77
5. Directional Nanoantennas
priori which magnetic and electric multipolar terms should be taken into account
in the expansion.
For a preliminary assessment of the orders of magnitude of each electric (al,m)
and magnetic (bl,m) multipolar coefficient, where m= -l, …, +l, we first obtained a
multipolar expansion of the antenna in free-space by direct numerical integration
of the simulated FDTD fields [84]. The results indicated that the emission of the
antenna is dominated by similar contributions by an electric dipole across the gap
(px), a magnetic dipole perpendicular to the SRR (mz) and two electric quadrupole
terms (Qxy= Qyx) with the rest of Cartesian components of the quadrupole
moment tensor equal to zero. Equivalently, this quadrupole is given in terms of
multipolar coefficients by a2,2= -a2,-2 with a2,0= a2,1= a2,-1= 0 [82].
With this simplification, it is now possible to reproduce the experimentally
observed angular patterns. We find, indeed, that the electric dipole, the magnetic
dipole and the electric quadrupole, all have a non-negligible contribution to the
radiation pattern (Fig. 5.15c); although the interferences of EQ-ED or MD-ED
alone already give directional patterns, only the combination of the three
reproduce all the features of the experimental angular pattern in Fig. 5.15a.
Conclusions
With a more compact, more broadband and more robust single-element design,
our magneto-electric antennas direct light emission comparably better than the
multi-element antennas of Sections 5.2 and 5.3. The volume of the antenna is only
λ3/200, the directional bandwidth is at least 200 nm and there is no need to
accurately position the emitters. Further tuning of the geometrical parameters
may result in higher directional and radiative enhancements. Interestingly, split-
ring resonators may be patterned by simpler nanofabrication methods such as
shadow-mask lithography because they do not require the alignment of multiple
elements. Therefore, these results are promising for the integration of directional
nanoantennas in light-emitting and light-harvesting devices.
From a fundamental point of view, the directional response of a SRR may be a
property to exploit in metamaterials. Understanding this directionality is
necessary to explain transmittance and absorption spectra commonly found in
experiments. For example, optical activity has been observed for achiral arrays of
SRRs under oblique incidence [196, 197]. This is a direct consequence of the
magneto-electric origin of the directionality of a single SRR.
78
6.
Antenna-Enhanced
Forbidden Transition
Spectroscopies
In previous Chapters, we have controlled the emission of electric
dipole electronic transitions with multipolar electromagnetic
antenna modes. Multipolar electronic transitions in the emitters
themselves, although usually slow compared to electric dipoles,
play a relevant role in various optical spectroscopies of several
materials. In this Chapter, through numerical simulations, we
evaluate and compare nanoantenna designs for the enhancement of
magnetic dipole and electric quadrupole transitions, while
simultaneously aiming to suppress electric dipole emission. We
identify promising geometries and materials suitable for the
experimental enhancement of forbidden-transition spectroscopies.
79
6. Antenna-Enhanced Forbidden Transition Spectroscopies
80
6.2 Enhancing forbidden transitions
Oxides. Certain spectral lines of oxides such as Cu2O and Cr2O3 are attributed
to electric-dipole-forbidden transitions [206, 207].
Atoms. The enhancement of an EQ transition in a vapor of atomic cesium was
reported under evanescent wave illumination of total internal reflection on
a dielectric interface [208].
Quantum dots and wires. In some semiconductor nanostructures, particularly
of larger sizes, non-ED effects have been measured for emission near a
mirror [209] and were also investigated theoretically [210, 211].
Molecular aggregates (J- and H-aggregates). Coherent coupling between
aligned molecular units can lead to non-dipolar contributions to
excitation, emission and energy transfer, because of the extended nature
of the excitonic wave function.
Raman and hyper-Raman spectroscopy. Raman vibration modes with
symmetries that have dipole-forbidden emission can potentially be
activated through EQ radiation by strong electric field gradients. This
electromagnetic mechanism has been suggested for the appearance of
certain Raman lines near metal nanoparticles [212, 213].
As in previous Chapters, angular measurements offer great potential to study the
multipolar nature of the interaction of light with matter, both in absorption and
in emission [214, 215]. In particular, back focal plane imaging can uncover non-ED
contributions in emission [130].
81
6. Antenna-Enhanced Forbidden Transition Spectroscopies
emitter may result in deletion of the excited state through another ED decay
channel. For an emitter at a given position on an antenna, a high branching ratio
between non-ED/ED transition rates is in principle desirable. Additionally, from a
practical point of view, it is preferable to have such a high enhancement and ratio
at all accessible points near the antenna.
Several nanostructures have been proposed recently for enhancing MD or EQ
optical transitions. Separate works evaluated the possibility of MD emission
control with metal nanowires [70], metal-insulator-metal resonators [221] and
semiconductor spheres [222-224]. For EQ transitions, independent theoretical
works predict enhancement by slits [225], metal spheres [213], dielectric spheres
[226], and gap antennas [227, 228].
In this Chapter, we provide a systematic evaluation and comparison of
different resonant antenna designs for MD and EQ enhancement: metal
nanospheres, metal nanowires, semiconductor disks, and split-ring resonators. We
identify geometries suitable for experimental realization, incorporating the effect
of surrounding media such as a dielectric substrate, and evaluating the possible
enhancement of ED transitions at the same or other emitter positions. The
presented simulations can therefore guide realistic experiments to manipulate
forbidden transitions.
Simulation method
We model the enhancement of non-ED transitions with classical electrodynamics.
Using the Finite-Difference Time-Domain method (FDTD Solutions, Lumerical
Inc.), we solve Maxwell’s equations numerically for MD and EQ sources. Our
approach is essentially similar to the study of ED enhancement by optical
antennas with the FDTD method [229]. By solving the full electromagnetic
problem in 3D, this method offers flexibility to study any nanoantenna design.
We compute the power radiated by an emitter coupled to an antenna, Prad, by
integrating the Poynting vector over a surface enclosing the emitter-antenna
system. The same emitter alone, without antenna and in vacuum, would radiate a
power Prad,0. We define the radiated power enhancement as the ratio Prad/Prad,0.
The radiated power enhancement relates directly to the radiative rate
enhancement: Prad/Prad,0= Γrad/Γrad,0. We will evaluate the performance of our
antennas in terms of this quantity.
We use mesh sizes of 1-3 nm and employ perfectly-matched layers at the
boundaries of the simulation volume. Temporal propagation is terminated when
the total power decays to 10-6 times the injected power for MD sources. For EQ
sources, the fields excited by a 20-fs pulse are propagated during a total of 200 fs
to ensure decay and convergence.
82
6.3 Magnetic dipole emission enhancement
For maximum accuracy, we place the electric and magnetic dipolar sources at
the positions of the mesh Yee cells where the respective fields are numerically
evaluated [230]. We construct EQ sources by adding two ED sources with the
same orientation 180° out of phase, separated by 1 nm. A finer refinement mesh
of 0.1 nm is used surrounding the EQ. The relative positions of the EDs
determine the resulting EQ, which can be of longitudinal or lateral character for
collinear or parallel dipoles, respectively. They correspond to the diagonal and off-
diagonal terms of the Cartesian quadrupole moment tensor (Qij with i, j= x, y, z).
As a general methodology, we simulate the emission of ED, MD or EQ sources
with different orientations and at different positions, normally 5 nm away from
the antenna surface. The resonance of each antenna is tuned by sweeping its
dimensions. In our results, we highlight the three most relevant situations: a non-
ED transition at its optimal position; an ED transition at the same position; and
an ED transition at its optimal position. For clarity, only dipole orientations with
maximum enhancement at each position are shown.
83
6. Antenna-Enhanced Forbidden Transition Spectroscopies
Metal-insulator-metal resonators
Another source of strong magnetic fields is the circulation of electric currents
between two parallel metal plates. Metal-insulator-metal (MIM) resonators
composed of cylindrical disks possess magnetic resonances that can be used for
ED emission enhancement [231]. For MD transitions, we obtain results that are
comparable in absolute value to a nanowire antenna (Fig. 6.1, center).
There are, however, important advantages. First, for an emitter placed at the
center of the resonator, where magnetic fields are maximal, the ratio of MD/ED
emission is significantly higher than for a nanowire (compare green and red
continuous lines). Second, the maximum MD enhancement is obtained for
orientations within the plane of the dielectric layer instead of a single direction.
As a result, the average enhancement will be higher for emitters with random
orientations. Third, although ED transitions display higher enhancement than
MD transitions at the rims of the resonator, the emitters may be contained only
inside the dielectric layer, making it easier in practice to position them towards
the center of the resonator. This might be accomplished, for example, by means of
radial chemical etching of the dielectric host material. MD enhancement is almost
constant with respect to the height of the emitter inside the resonator, providing
an extended volume for emission enhancement (Fig. 6.2, center).
85
6. Antenna-Enhanced Forbidden Transition Spectroscopies
Semiconductor resonators
Semiconductor and dielectric nanospheres and nanowires exhibit magnetic
resonances [97-99] that may be used for the enhancement of MD transitions. They
support low-order Mie resonances whose local magnetic field distribution is
maximal at its center. Here, we evaluate a related antenna geometry that might
be more controllably used in experiments; a cylindrical silicon disk on a substrate.
Enhancement factors can be above 100 at near-infrared wavelengths for MD
dipoles centered and perpendicular to the top surface of the silicon disks (Fig. 6.1
for a disk on a glass substrate; Fig. 6.2 for a disk on a silicon-on-insulator
substrate). At that position, the contrast of MD/ED enhancement can exceed 20
times. Importantly, an ED is only weakly enhanced at other positions around the
resonator, e.g., at the side or at the edges.
Although other dielectric materials with a lower —yet relatively high—
refractive index still support similar magnetic resonances, the enhancement is
smaller [222]. By simulating disks made of diamond (n≈ 2.4) and TiO2 (n≈ 2.7),
we found enhancements of MD transitions below 30 at the studied wavelengths.
The higher refractive index of semiconductors such as Si (n≈ 3.6) contributes to a
stronger resonant enhancement.
Split-ring resonators
The curvature of the electric current in a resonant split-ring resonator produces
strong magnetic fields, especially near its curved section. We evaluate next MD
enhancement with a U-shaped resonator (SRR), similar in geometry to a tuning
fork, whose arms can be tuned into resonance by varying their length.
The first resonant mode of a SRR in air offers a high enhancement of both ED
and MD transitions (Fig. 6.3, left). However, the antenna dimensions are small
even when surrounded only by air, and even smaller geometries would be required
for antennas on a realistic glass substrate. Larger split-ring resonators exhibiting
higher-order resonances may be considered for ease of fabrication, including a
glass substrate. We find, however, that the MD enhancements achievable with
higher-order modes on a substrate are considerably lower and provide a lower
contrast of MD/ED enhancement (Fig. 6.3, right).
Finally, we also simulated other structures known to support magnetic
resonant modes —including nanoslot antennas, parallel wire pairs, and
metal/dielectric core-shell resonators— and found no evidence of performance
superior to, for example, a nanowire antenna.
86
6.4 Electric quadrupole emission enhancement
Metal spheres
A noble metal sphere with a nanoscale radius provides a basic combination of
field gradients and resonant emission. Although the resonance of the antenna can
still be identified, our simulations show that there is a relatively constant level of
non-resonant enhancement throughout the spectrum (Fig, 6.4, left).
A longitudinal quadrupole with dipoles oriented along the radius of the sphere
can be enhanced by more than 3 orders of magnitude as a result of field gradients
of the form ∇xEx. The different local fields seen by each dipole break the
symmetry of the emitter producing more radiation.
87
6. Antenna-Enhanced Forbidden Transition Spectroscopies
Figure 6.4 Antennas for electric quadrupole transitions. The field gradients
near a gold sphere and a nanowire can enhance the radiative rates of quadrupolar
transitions by several orders of magnitude. In both cases, the enhancement is
much higher than for ED sources. Two types of quadrupoles are compared, lateral
and longitudinal, with constituting dipoles at different relative positions. All
sources are 5 nm away from the antenna surface.
Metal nanowires
A nanowire antenna may have sharper edges than a sphere, producing steeper
field gradients as well as higher resonant local fields. The result is that an EQ
transition is enhanced by more than 4 orders of magnitude. The resonance of the
antenna is clearly visible in the spectrum of Figure 6.4, with similar shapes for ED
and EQ sources. Interestingly, ED emission is enhanced by at least 2 orders of
magnitude less than EQ transitions.
88
6.5 Conclusions
Figure 6.5 Field gradients near edges for quadrupolar transitions. The
power radiated by a quadrupole transition increases near antennas features of
small radius of curvature, such as smaller spheres (diameter, D) or the sharper
edges of a nanowire (position of the emitter with respect to the center height of
the nanowire, z).
6.5. Conclusions
We have demonstrated through numerical simulations the feasibility of enhancing
magnetic dipole and electric quadrupole transitions with resonant optical
antennas. The antenna mode does not need to have the same multipolar character
as the transition, as illustrated with nanowire ED antennas and both MD and EQ
sources. With realistic configurations and potentially working at other
wavelengths, our results can serve as a guide to a range of spectroscopic
experiments.
The observable effects of the activation of forbidden transitions by optical
antennas will depend on the enhanced optical process. Experimental signatures of
such enhancement could be the spectral modification of an emitter through the
appearance or suppression of spectral lines, the shortening of a decay lifetime, or a
signal intensity enhancement.
89
6. Antenna-Enhanced Forbidden Transition Spectroscopies
90
Conclusion
In this Thesis, we have demonstrated the control of light emission with optical
antennas. The near-field coupling of an emitter to a tailored nanoantenna resulted
in controlled directions of emission, polarization, decay rate or wavelength
spectrum. Each antenna design conferred its properties on the emitter,
dominating the emission.
Nanowire antennas produced multipolar radiation from dipolar transitions,
acting as converters between fundamental electromagnetic modes with different
symmetries. Nanoslot antennas were shown to possess a dominant magnetic dipole
response at resonance, even when driven by electric dipole sources. Yagi-Uda and
log-periodic antennas directed light emission through the interference of dephased
electric dipoles. Judiciously tuned split-ring resonators made unidirectional
emission possible with a single, compact element through interfering multipolar
moments. Finally, we explored the possibility of enhancing multipolar transitions
in the emitters themselves with optical antennas of arbitrary multipolar character.
Our antennas were mainly inspired by conventional antenna designs. There is
still plenty of room for ideas and improvement to be drawn by the optical
antenna engineer from that vast body of knowledge. Yet, designs exclusive to
optical frequencies might be found that outperform classical ones, as illustrated in
our example of magneto-electric antenna (split-ring resonator). Those potential
designs might be more suited to the peculiarities and applications of optical
antennas.
Research in optical antennas is full of opportunities for integration in photonic
devices. For example, directional antennas can couple light into dielectric,
semiconductor or plasmonic waveguides. A coherent communication link between
two independent emitters with optical antennas has yet to be demonstrated; it
could boost the prospects for nanophotonic wireless networks. The combination of
nanoantennas with micro/nano-fluidics has the potential to revolutionize
biochemical sensors. The control of the electromagnetic modes of emission and
absorption enabled by optical antennas provides interesting opportunities to
91
manipulate the orbital angular momentum of light with sub-wavelength sources
and detectors, ideal for integration in more complex devices.
Light emission can still be more radically manipulated with optical antennas.
Breaking the selection rules through the enhancement of multipolar transitions
with optical antennas seems certainly within experimental reach, as shown in the
simulations in this Thesis. For dipolar transitions, our work always took place in
the weak-coupling regime. Access to the strong-coupling regime would allow the
use of quantum electrodynamics effects as a resource for optoelectronics. Also for
dipolar emitters, emission and excitation enhancements reported in the
experimental literature are still far from the values predicted by theory. If the
enhancements expected for gap antennas are obtained, they would enable the
detection of very slow emitters such as single rare-earth ions. Such emitters would
constitute virtually unbleachable solid-state sources of single photons for quantum
information technologies. The enhancement of these and other emitters could be
combined with spin manipulation.
This Thesis provided part of the necessary groundwork for these and other
exciting experiments by establishing the fundamental methods and the Optical
Physics of antennas as nano-optical elements.
92
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List of Publications
Book Chapter
“Directionality, polarization and enhancement by optical antennas”
N. F. van Hulst, T. H. Taminiau, and A. G. Curto,
Optical Antennas, Eds. M. Agio and A. Alù, Cambridge University Press (2013)
Journal Articles
“Antenna-Enhanced Forbidden Transition Spectroscopies”
A. G. Curto, M. Kuttge, and N. F. van Hulst,
In preparation
“Magneto-Electric Antennas for Directing Light Emission”
I. M. Hancu, A. G. Curto, M. Castro-Lopez, M. Kuttge, and N. F. van Hulst,
In preparation
“Probing the Magnetic Resonance of a Nanoslot Optical Antenna”
A. G. Curto, M. Kuttge, N. F. van Hulst
Under review in Physical Review Letters (2013)
“Multipolar Radiation of Quantum Emitters with Nanowire Optical Antennas”
A. G. Curto, T. Taminiau, G. Volpe, M. Kreuzer, R. Quidant, N. F. van Hulst,
Nature Communications 4, 1750 (2013)
“Log-Periodic Optical Antennas with Broadband Directivity”
R. S. Pavlov, A. G. Curto, N. F. van Hulst,
Optics Communications 285, 3334–3340 (2012)
“Unidirectional Emission of a Quantum Dot Coupled to a Nanoantenna”
A. G. Curto, T. Taminiau, G. Volpe, M. Kreuzer, R. Quidant, N. F. van Hulst,
Science 329, 930-932 (2010)
“Near-Field Focusing with Optical Phase Antennas”
A. G. Curto, A. Manjavacas, and F. J. García de Abajo,
Optics Express 17 (20), 17801-17811 (2009)
“Near-Field Optical Phase Antennas for Long-Range Plasmon Coupling”
A. G. Curto and F. J. García de Abajo,
Nano Letters 8 (8), 2479-2484 (2008)
Other Publications
“Optical Antennas for Quantum Emitters”
A. G. Curto, M. Castro-Lopez, and N. F. van Hulst
Óptica Pura y Aplicada 44 (2) 325-331 (2011)
109