Letter

pubs.acs.org/NanoLett

Transient Reflection: A Versatile Technique for Ultrafast

Spectroscopy of a Single Quantum Dot in Complex Environments
Christian Wolpert,†,§ Christian Dicken,†,§ Paola Atkinson,‡ Lijuan Wang,‡ Armando Rastelli,‡
Oliver G. Schmidt,‡ Harald Giessen,† and Markus Lippitz*,†,§
†
4th Physics Institute and Research Center SCOPE, University of Stuttgart, Pfaffenwaldring 57, D-70550 Stuttgart, Germany
‡
Institute for Integrative Nanosciences, IFW Dresden, Helmholtzstrasse 20, D-01069 Dresden, Germany
§
Max Planck Institute for Solid State Research, Heisenbergstrasse 1, D-70569 Stuttgart, Germany
*
S Supporting Information

ABSTRACT: Increasingly complex structures such as optical

antennas or cavities are coupled to self-assembled quantum
dots to harvest their quantum-optical properties. In many
cases, these structures pose a problem for common methods of
ultrafast spectroscopy used to write and read out the state of
the quantum dot. We present a pure far-field method that only
requires optical access to the quantum dot and does not
impose further restrictions on sample design. We demonstrate
Rabi oscillations and perturbed free induction decay of single
GaAs quantum dots that have a dipole moment as small as 18 D. Our method will greatly facilitate ultrafast spectroscopy of
complex quantum-optical circuits.
KEYWORDS: Coherent spectroscopy, quantum emitter, plasmonic nanocircuits

S emiconductor quantum dots (QDs) closely resemble

atomic dipole emitters in the solid state,1 which makes
them attractive building blocks for novel photonic devices. We
can individually address, manipulate and read them out on
picosecond time scales using ultrafast spectroscopy.2 Individual
dots already find use as single photon sources for quantum
cryptography3 or as quantum bits for quantum computing.4
Hybrid quantum systems combining a quantum dot with a
microcavity5,6 or a particle plasmon7−10 can enhance light-
matter interaction. Even more fascinating applications require
the controlled interaction of many quantum systems in a
network. Recent publications envision the entanglement of
quantum dots by means of plasmonic waveguides11 or the use
of quantum dots as optical transistors.12
To realize these proposals, one needs to fulfill at least two
requirements, namely the controlled positioning of the emitter
relative to the nanostructure and ultrafast optical spectroscopy
on the combined system. The first point can be realized by
using self-assembled quantum dots that grow at positions
defined by electron-beam lithography.13,14 The second require-
ment needs a noninvasive optical technique that does not
interfere with the structure around the quantum dot. Optical
far-field spectroscopy is such a technique. It has been
successfully applied to ultrafast coherent spectroscopy of
interface-fluctuation quantum dots (for a review see ref 2).
However, these stochastically formed dots are not compatible
with methods of deterministic positioning. Self-assembled
quantum dots, in contrast, can be grown in a site-controlled
manner, but in turn have a much smaller absorption cross-
section. In order to overcome the weak light-matter interaction,
researchers resorted to nanoapertures to block unwanted
light,15,16 to electrodes that modulate the emission line by
the Stark shift,17 or to collecting the electrons tunneling out of
the quantum dot.18 All these approaches hinder or even make
impossible the fascinating plasmonic nanocircuit applications as
discussed above. In this Letter, we demonstrate that far-field
reflection spectroscopy is appropriate to gain ultrafast
spectroscopic information of single quantum dots without
further restrictions to the structure design. This allows for the
first time experiments with quantum dots in complex systems.
We first introduce our experimental technique and then
demonstrate its capabilities on two classical examples of
ultrafast spectroscopy of quantum emitters, namely Rabi
oscillations19,20 and perturbed free induction decay.21−23
Concept. The key idea (see Figure 1A) is that the
absorption by a dipole can be understood as the interference
of the optical wave scattered at the dipole in forward direction
with that passing the dipole unperturbed, known as the optical
theorem.24 Both absorption and reflection have their origin in
the scattered field ES of a dipole25
α0 −i γ
ES = α̃ (ω)E0 with α̃ (ω) =
2 δ + iγ (1)
Received: October 28, 2011
Revised: December 2, 2011
Published: December 15, 2011

© 2011 American Chemical Society 453 dx.doi.org/10.1021/nl203804n | Nano Lett. 2012, 12, 453−457
Nano Letters
Figure 1. (A) The field scattered at the quantum dot interferes with
the transmitted as well as with the reflected probe field. It gives rise to
transient absorption and transient reflection features. (B) The phase
lag ϕ changes the spectral line shape of the transient reflection signal
from absorptive to dispersive and back.
where E0 is the exciting probe field, α0 is the peak absorption of
the dipole, δ = ω − ω0 is the probe detuning from the dipole’s
resonance, and γ ≪ ω0 is the resonance width. The total
transmitted and reflected fields are the respective coherent
sums of the scattered field with the unperturbed transmitted or
reflected probe fields, taking the Fresnel coefficients for
reflection and transmission, r and t, of the sample surface
into account.25
E T = tE0 + α̃ (ω)tE0
ER = rE0 + α̃ (ω)ei2ϕt 2E0
ϕ describes the phase lag that the field acquires by traveling
from the sample surface to the dipole position. The phase lag ϕ
influences the spectral shape of the signal, varying from an
absorptive to a dispersive line shape, as shown in Figure 1B .
This interference effect was used to detect single molecule
absorption,26 steady-state absorption of single quantum dots,27
and transient absorption of single interface-fluctuation quantum
dots using a scanning near-field aperture23 or heterodyne
spectral interferometry.28 We will apply this technique to
ultrafast spectroscopy of a weakly absorbing self-assembled
quantum dot.
Sample. Our quantum emitters are epitaxial GaAs quantum
dots in AlGaAs barriers.29 The dots form in self-assembled
nanoholes that were prepared at low density in the lower
AlGaAs layer. Detailed structural information is provided in the
Supporting Information. The fundamental transition of the
localized exciton is around 1.7 eV where the quantum efficiency
of Si-based photodetectors is high. The asymmetry of the
quantum dot leads to linear polarization selection rules and a
fine structure splitting (FSS) in the order of 100 μV between
the two fundamental bright exciton states, which we denote as
|01⟩ and |10⟩ (see inset in Figure 2 and ref 30). The
polarization directions, Π90° and Π0°, are oriented along the
crystal axes [11̅0] and [110]. The GaAs substrate is situated
only 20 nm below the QD layer. It absorbs at the exciton
resonance energy. This complex environment makes a
traditional transient transmission experiment impossible.
Experiment. Orthogonally polarized pump and probe
pulses at the exciton resonance wavelength are derived from
a mode-locked Ti:Sapphire laser in combination with two
spectral pulse shapers. This results in a temporal resolution of
1 ps. The temporal delay Δt between both pulses is varied by a
mechanical translation stage. The collinear beams are focused
by a 0.7 NA objective onto the sample in a cryostat (T = 10 K).
The spatial resolution is in the order of 700 nm, which allows
us to address single quantum dots. The reflected probe light is
collected by the same objective and analyzed by a spectrometer
Letter
Figure 2. Spectrum of the reflected probe light R(ω,Δt) in the
presence of the pump (blue curve) and after subtraction of the
reference spectrum (no pump): ΔR = R(ω,Δt) − R0(ω) (red curve).
The energy scale is relative to the exciton energy of the quantum dot
at 1.72 eV. The pump−probe delay was set to Δt = 150 ps. Pump-
induced bleaching of the exciton transition in the QD is responsible
for the sharp feature at zero detuning. The noise is limited by photon
shot noise to 2.4 × 105 photons, resulting in a signal-to-noise ratio of
about 17 with an integration time of 10 min. Inset: Energy level
diagram of the fundamental transition of a quantum dot. The excitonic
states |10⟩ and |01⟩ are separated by the fine structure splitting (FSS),
(2) while the biexciton state |11⟩ is reduced in energy due to Coulomb
interaction.
(3) equipped with a CCD camera (spectral resolution 100 μeV).
The reflected pump light in turn is suppressed by crossed
polarizers and a double modulation scheme. The high quantum
efficiency of the CCD camera allows us to acquire shot-noise
limited reflection spectra with more than 1010 photons per pixel
in one minute integration time. In addition, fluorescence
emission spectra and spatial emission maps can be taken.
Details on experimental parameters and data processing can be
found in the Supporting Information.
The transient reflection spectrum ΔR/R of a single quantum
dot is acquired by taking the difference of the probe reflection
spectrum with and without preparing an excited state by the
pump pulse. The pump and probe beams are switched on and
off independently by acousto-optic modulators at a rate of
1 kHz. By subtracting consecutive spectra from each other,
differential reflection spectra are obtained which are then
normalized to the spectrum of the probe pulse.
Figure 2 shows an example of the probe spectrum R(ω,Δt)
(blue curve) and the difference of subsequent spectra
ΔR(ω,Δt) (red curve) as a function of the detuning ΔE from
the fundamental exciton transition in a single quantum dot.
One can discern two contributions to ΔR: a spectrally broad
signal that reproduces the shape of the probe spectrum and a
sharp, dispersive feature at the exciton transition energy. The
broad signal originates from a modified reflectivity due to the
presence of photocarriers created by band absorption in the
GaAs substrate and cap.31,32 As the distance of the quantum dot
to the sample surface corresponds to a phase lag ϕ = 0.2 π
(Figure 1B), we find a dispersive spectral feature from the
quantum dot at the exciton resonance. This sharp contribution
to the spectrum is due to bleaching of the |00⟩ → |01⟩
transition (see inset in Figure 2). When the pump pulse
populates state |10⟩, the transition |00⟩ → |01⟩ cannot be
driven by the probe pulse. The amplitude of the dispersive
feature therefore monitors the population n10 of state |10⟩. We
fit the line shape25,33 and obtain a zero-to-peak amplitude of
ΔR/R = 5.0 × 10−5. In comparison to steady-state frequency
resolved experiments,25 in the present experiment the signal
454 dx.doi.org/10.1021/nl203804n | Nano Lett. 2012, 12, 453−457
Nano Letters
amplitude is reduced by the ratio of the quantum dot line width
(several μeV) to the resolution of our spectrometer (100 μeV).
In spite of this reduction, Figure 2 demonstrates that plain far-
field reflection spectroscopy is able to measure transient signals
of a single quantum dot.
Rabi Oscillations. Let us turn now to coherent spectros-
copy of the quantum dot’s exciton transition. We manipulate
the state of the quantum dot by a pump pulse which is resonant
with the |00⟩ → |10⟩ transition. The pulse can drive the
quantum dot to the |10⟩ state and, as it is shorter than the
coherence time of that transition, also back again to the ground
state, leading to Rabi oscillations in the population n10
proportional to sin2(θP/2). The pump pulse area θP is
proportional to the square root of the pump intensity
∞ EP⃗ (t ) ·μ⃗
θP = ∫−∞ ℏ
dt
(4)
where E⃗ P(t) is the electric field of the pump pulse at the site of
the quantum dot and μ⃗ is the transition dipole moment of the
exciton. The system is completely inverted for a pulse with
θP = π (π-pulse), whereas a 2π-pulse performs a full rotation
and leaves the system in the ground state.
As described above, we monitor the population n10 by the
bleaching it imposes on the |00⟩ → |01⟩ transition. In the
spectral map (Figure 3A) every vertical line is a ΔR/R spectrum
Figure 3. (A) Each vertical cut through the color map represents a
ΔR/R spectrum at a given pump power and a fixed pump−probe delay
Δt = 150 ps. The broad background has been subtracted. (B) By
fitting the dispersive line shape function to the spectra in (A), the
signal amplitude (blue dots) is extracted. The error bars are the
standard deviation of four consecutive measurements. The scale of the
pump pulse area θp is calibrated to the first maximum. The data can be
described by sin2(θ/2), considering an effective, reduced pulse area θeff
due to delocalized carriers around the quantum dot (red curve).
at a certain pump power. In Figure 3B, the signal amplitudes
are extracted from the spectra by fitting a dispersive line shape
function to the spectral data. Two complete cycles of the Rabi
oscillation are visible. In contrast to the textbook example, they
show a gradual stretching of the oscillation period. We find the
origin of this stretching in the carriers that the pump pulse
creates in the GaAs layers near the quantum dot. The density of
these carriers influences the overall reflectivity of the sample
and thus is responsible for the broad background signal34,35
(Figure 2). This signal follows a saturation law from which we
can determine a saturation power Psat from it (see Supporting
Information). Using this saturation power, we can fully describe
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Letter
the data by considering an effective pulse area θeff
⎛ P ⎞
⎜ ⎟
Psat
θeff = θP⎜1 − f ⎟
P
⎜ 1+ ⎟
⎝ Psat ⎠ (5)
where P and f are the pump power and a free fitting parameter,
respectively. This relation between the bulk carrier concen-
tration and the pump pulse area reduction points to an effect
on a picosecond time scale, as the probe pulse coming at least
50 ps later is unmodified (the height of the Rabi oscillations is
constant). Simultaneously, no free carriers relax into the
quantum dot, as the Rabi oscillation returns to zero. The
microscopic origin of this effect is under current investigation.
Taking into account all experimental parameters that can be
determined independently (see Supporting Information) the
only remaining fitting parameters in Figure 3B are the
transition dipole moment |μ⃗|, the proportionality factor f, and
an overall amplitude scaling parameter. As the dipole moment
enters both the signal amplitude (via α0 in eq 1) as well as the
pump pulse area (via eq 4) the amplitude scaling factor in the
order of one only accounts for experimental imperfections.
To evaluate the stability and reproducibility of our
measurement scheme, we varied the delay time Δt from 50
to 200 ps (details in the Supporting Information). The signal
shows no dependence on the pump−probe delay but a minor
reduction in amplitude due to the finite lifetime of the exciton.
Comparing several quantum dots we obtained transition dipole
moments |μ⃗| between 17 and 19 D. The saturation intensities
varied between 150 and 600 MW/cm2, which is in good
agreement with the literature values for defect-rich GaAs.36,37
The values of the fitting parameter f varied between 0.5 and 0.8.
The considerable range of these two parameters describing the
delocalized carriers suggests that the environment of the
different quantum dots is not very uniform. The transition
dipole moments are, however, almost unaffected by the
differing environments. This underlines the strength of optical
spectroscopy on the level of single nanoobjects.
Perturbed Free Induction Decay. While the Rabi
oscillations were measured as a function of pump power, we
can also follow the dynamics of the exciton in the time domain.
A classical example is the perturbation of the free induction
decay by the pump pulse.21−23 In a density matrix picture the
probe pulse creates coherence between the states |00⟩ and |01⟩.
The exponential decay of the coherence leads via Fourier
transform to the Lorentzian spectral line of the scattered light.
When a pump pulse (coming after the probe pulse) perturbs
the decay of the coherence in some way, the spectral shape
changes, resulting in a differential reflection signal ΔR/R.
Figure 4 presents transient reflection spectra for pump−
probe delays varying from −30 ps to +30 ps. Positive delays
describe a pump pulse that precedes the probe pulse, as was
used to acquire Rabi oscillations where the pump pulse depletes
the ground state. We find a dispersive spectral feature that
decays with the exciton lifetime on a 200 ps time scale. As in
previous work,21−23 for negative delays the spectra show fringes
that separate further with reducing pump−probe delay,
resulting in hyperbolic features.
The whole data set can be simulated using a density matrix
model of only three levels (|00⟩, |01⟩, |10⟩) that are optically
connected in a V shape. We find perfect agreement in all details
when taking into account the interference of the scattered and
reflected probe field. The only free fitting parameters are the
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Nano Letters
Figure 4. (Top) Differential spectra as a function of pump−probe
delay in experiment and simulation. (Bottom) Temporal evolution of
the probed exciton polarization for the probe preceding the pump
pulse (negative delays, left figure) and the probe arriving after the
pump pulse (positive delays, right figure). In the first case, the pump
perturbs the polarization, leading to spectral fringes. In the second
case, the pump depletes the ground state, reducing the probed
polarization.
coherence time T2 = 90 ps and the lifetime T1 = 230 ps of the
probed transition (for details see the Supporting Information).
In the density matrix model, the scattered probe field equals
the imaginary part of the matrix element ρ|00⟩ |01⟩, describing the
probed exciton polarization. The lower row of Figure 4 depicts
examples of the temporal evolution for negative and positive
pump−probe delay. For positive delay the pump pulse bleaches
the ground state |00⟩ so that less polarization is built up,
resulting in a weaker scattered field and a dispersive feature in
the transient reflection spectrum. For negative pump−probe
delays, the decay of the polarization is perturbed by the pump
pulse as it bleaches the ground state. The resulting polarization
trace can be seen as the sum of a reduced free induction decay
(dashed line in Figure 4C) and a rectangle with a width equal
to the pump−probe delay (shaded area in Figure 4C). The
latter leads by Fourier transform to the fringes in the spectral
domain. Like in the case of Rabi oscillations, this example
demonstrates again the advantage of a spectrally resolved
experiment. Only the rich information content of the
differential spectra makes it possible to distinguish between
the quantum dot signal, perturbed free induction decay, and
background contributions.
Conclusion. We demonstrated that simple far-field
reflection spectroscopy is sufficient to determine the ultrafast
dynamics of a single self-assembled quantum dot. As one
example, we determined the dipole moment of strain-free GaAs
quantum dots on an absorbing substrate by Rabi oscillations to
be 17−19 D. We also showed spectrally resolved perturbed free
induction decay of a localized exciton in full agreement with a
density matrix model involving only a three level V-system. We
expect our method to find applications in ultrafast coherent
spectroscopy of complex quantum-optical structures, such as
quantum emitters in photonic or plasmonic circuits. Without
any further requirements on the sample design, the transient
spectra contain enough information to separate the individual
contributions of the quantum dot and the nanoenvironment
456
Letter
and the effect of their coupling. Similar to the spectral signature
of the delocalized carriers presented above, the response of any
nanoenvironment can be taken into account when modeling
the coupled system. Transient reflection spectroscopy is not
limited to epitaxial samples. Colloidal nanocrystals or even
molecules could be investigated when prepared on a partially
reflecting substrate such as a cover slide. Our technique will
make coherent experiments feasible in a large group of
structures where other techniques are very difficult or
impossible to apply.
■
*
ASSOCIATED CONTENT
S Supporting Information
Growth of the GaAs/AlGaAs quantum dots. Details on the
experimental setup. Additional data sets for Rabi oscillations
and the background contribution. Density matrix model for a
V-system and calculation of differential reflectivity spectra.
Additional corresponding references. This material is available
free of charge via the Internet at http://pubs.acs.org.
■
AUTHOR INFORMATION
Corresponding Author
*E-mail: m.lippitz@physik.uni-stuttgart.de.
■
ACKNOWLEDGMENTS
Our research was supported by the Deutsche Forschungsge-
meinschaft DFG (research unit FOR 730) and the Baden-
Württemberg Stiftung.
■
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