Self-assembled InGaAs Quantum Dots Research Articles

Temperature dependent temporal coherence of metallic-nanoparticle-induced single-photon emitters in a WSe2 monolayer

In recent years, much research has been undertaken to investigate the suitability of two-dimensional materials to act as single-photon sources with high optical and quantum optical quality. Amongst them, transition-metal dichalcogenides, especially WSe2, have been one of the subjects of intensive studies. Yet, their single-photon purity and photon indistinguishability remain the most significant challenges to compete with mature semiconducting systems such as self-assembled InGaAs quantum dots. In this work, we explore the emission properties of quantum emitters in a WSe2 monolayer which are induced by metallic nanoparticles. Under quasi-resonant pulsed excitation, we verify clean single-photon emission with a g (2)(0) = 0.036 ± 0.004. Furthermore, we determine the temperature dependent coherence time via Michelson interferometry, where a value of (13.5 ± 1.0) ps is extracted for the zero-phonon line at 4 K, which reduces to (9 ± 2) ps at 8 K. Associated time-resolved photoluminescence experiments reveal a decrease of the decay time from (2.4 ± 0.1) ns to (0.42 ± 0.05) ns. This change in decay time is explained by a model which considers a Förster-type resonant energy transfer process which yields a strong temperature induced energy loss from the single-photon emitters to the nearby Ag nanoparticle.

Effect of bismuth surfactant on the structural, morphological and optical properties of self-assembled InGaAs quantum dots grown by Molecular Beam Epitaxy on GaAs (001) substrates

In this work, we have investigated the effect of Bi surfactant on structural, morphological and optical properties of 5 monolayers self-assembled InGaAs quantum dots (QDs) grown on GaAs (001) substrates at various growth temperatures (435, 467 and 495 °C) by Molecular Beam Epitaxy. Two types of InGaAs QDs samples grown with and without exposure to bismuth were studied using Atomic Force Microscopy, Scanning Electron Microscopy, Transmission Electron Microscopy and Photoluminescence (PL). Our results have demonstrated that Bi-mediated growth provides improved control of several properties of InGaAs QDs including an enhancement of the QD PL peak intensity by 1.7 times as compared to InGaAs/GaAs control sample grown without Bi. In addition, a red-shift of the PL peak energy of about 40 meV was also observed when the InGaAs QDs were grown by using Bi evidencing that Bi surfactant affects considerably the size of QDs. Furthermore, the QDs grown with Bi surfactant exhibited a higher degree of size uniformity as demonstrated by the observation of narrower Full Width at Half Maximum (FWHM) of the PL peaks. We have also shown that both Bi surfactant and substrate temperature play an important role to control the density of InGaAs QDs. The QD density decreased from 8.9 × 1010 cm−2 (control sample) to 2.0 × 1010 cm−2 for the sample grown at the lowest temperature of 435 °C under Bi flux. All these approaches to control and improve the properties of self-assembled QDs are important for device applications that require high optical efficiency and low QD density.

Dark-bright excitons mixing in alloyed InGaAs self-assembled quantum dots

Quantum dots are arguably one of the best platforms for optically accessible spin based qubits. The paramount demand of extended qubit storage time can be met by using quantum-dot-confined dark exciton: a longlived electron-hole pair with parallel spins. Despite its name the dark exciton reveals weak luminescence that can be directly measured. The origins of this optical activity remain largely unexplored. In this work, using the atomistic tight-binding method combined with configuration-interaction approach, we demonstrate that atomic-scale randomness strongly affects oscillator strength of dark excitons confined in self-assembled cylindrical InGaAs quantum dots with no need for faceting or shape-elongation. We show that this process is mediated by two mechanisms: mixing dark and bright configurations by exchange interaction, and equally important appearance of non-vanishing optical transition matrix elements that otherwise correspond to nominally forbidden transitions in a non-alloyed case. The alloy randomness has essential impact on both bright and dark exciton states, including their energy, emission intensity, and polarization angle. We conclude that, due to the atomic-scale alloy randomness, finding dots with desired dark exciton properties may require exploration of a large ensemble, similarly to how dots with low bright exciton splitting are selected for entanglement generation.

Fine structure of dark and bright excitons in vertical electric fields: Atomistic theory of alloyed self-assembled InGaAs quantum dots

The vertical electric field response of dark- and bright-excitonic fine structures in self-assembled quantum dots remains largely unexplored. Using an atomistic tight-binding model, combined with a configuration-interaction approach, we show that the fine structure of both bright and dark excitons can be effectively tuned with a vertical field. The dark-exciton splitting reveals parabolic evolution under an applied electric field, contrary to linearlike trends for the bright-exciton splitting, with a linear change rate of the latter related to the bright-dark splitting. Atomistic results are further investigated in terms of the hole-band-mixing term, which reverses its sign under the electric field leading to a vanishing bright-exciton fine structure, and a minimum of the dark-exciton splitting in a nonalloyed case. Surprisingly, we find that the dark-exciton optical activity is also highly tunable with the electric field, despite the quantum dot's cylindrical shape, with potential implications for applications involving dark excitons. Finally, we study different random realizations of the same alloyed quantum dot, showing that mere alloy randomness substantially affects the bright-exciton splitting both at zero field and at the splitting minimum.

Perspective of self-assembled InGaAs quantum-dots for multi-source quantum implementations

In recent years, semiconductor quantum dots have demonstrated their potential to reach the goal of being an ideal source of single and entangled photon pairs. Exciting reports of near unity entanglement fidelity, close to unity photon indistinguishability, and high collection efficiency in nanophotonic structures have been demonstrated by several distinct groups, showing unequivocally the maturity of this technology. To achieve the required complexity and scalability in realistic quantum photonic implementations, two-photon interference of photons from multi-sources must be reached. While high indistinguishability values have been observed for photons generated from the same source within a relatively short time separation, achieving similar visibility for larger time separation or in multi-source experiments still requires intensive efforts. In fact, the coupling to the particular mesoscopic environment of charge carriers confined in the quantum dot leads to decoherence processes, which limit the quantum interference effects to a short time window. Here, we discuss the progress in studying the dynamics of this decoherence, which crucially depends on the evolution of line broadening in high-quality self-assembled InGaAs quantum dots. Characterization of line broadening mechanisms is the first fundamental step to be able to counteract them. Optimization of the growth and active and passive control of the radiative transitions are crucial for the technological readiness of non-classical light sources based on semiconductor platforms.

InGaAs quantum dots-in-a-well solar cells with anti-reflection coating

To improve the performance of self-assembled InGaAs quantum dots (QDs) solar cells, we introduce a 2-nm In0.1Ga0.9As quantum well underneath each In0.75Ga0.25As QDs layer to form an InGaAs quantum dots-in-a-well (DWell) structure. The coupled DWell solar cell consists of nine DWells spacing by GaAs layers. We change the GaAs spacer thickness to optimize the photovoltaic performance. The solar cell of 15-nm GaAs spacer shows the best results, including the open-circuit voltage (VOC) = 0.67 V, the short-circuit current density (JSC) = 17.4 mA/cm2, and the power conversion efficiency (η) = 8.7%, compared to the coupled InGaAs QDs counterpart of VOC = 0.59 V, JSC = 18.6 mA/cm2, and (η) = 8.0%. The enhancement of VOC for the DWell solar cell is attributed to the lower dark saturation current, which is caused by stronger carrier confinement and lower strain-induced defects in the active region. The DWell solar cell is further improved by Al2O3/HfO2 anti-reflection coating, and reaches η = 11.8% as JSC increases to 23.5 mA/cm2.

Correlation between photoluminescence and morphology for single layer self-assembled InGaAs/GaAs quantum dots

Single layer self-assembled InGaAs quantum dots (QDs) are manipulated by using different arsenic species on GaAs (100) surface. The As4 molecules are experimentally observed to be more promising than As2 to promote the formation of one-dimensionally-aligned QD-chain arrays. The lateral alignment of QDs and the corresponding formation of dot chains are explained by the anisotropic surface kinetics in combination with the different reactivities of the two molecules with bonding sites on the GaAs (100) surface. Photoluminescence (PL) measurements demonstrate that the spectra of the QD-chains broaden to higher energy and increases in intensity with increasing excitation laser power. The PL band of the QD-chains also exhibits a 9 meV reduction in linewidth as temperature increases starting from 8 K. These observations confirm an efficient lateral coupling between neighboring QDs and thereafter polarized QD emission, whereas the randomly distributed QDs grown with As2 show no preferential polarization. Such QD-chains exhibiting anisotropic properties have the potential for nanophotonics applications like electro-optic modulators with very low drive voltage and ultra-wide bandwidth operation.

Investigation of multimodality effect in quantum dots InGaAs/GaAs grown by MOVPE

Self-assembled InGaAs quantum dots with In content 80% grown on vicinal GaAs substrates by MOVPE method have been investigated by photoluminescence technique in a wide range of temperatures and excitation densities. Multimodality of distribution of size and (or) shape in array of vertically stacked quantum dots synthesized under different growth conditions as well as in a single layer structure was found on the ground of appearance of a set of peaks in photoluminescence spectra at lowered temperatures. Influence of growth conditions on density and radiation wavelength of quantum dot modes has been analyzed. Investigation of photoluminescence of samples as a function of temperatures has allowed determining activation energies of three channels of the losses that were attributed to different modes of quantum dots.

Narrow optical linewidths and spin pumping on charge-tunable close-to-surface self-assembled quantum dots in an ultrathin diode

We demonstrate full charge control, narrow optical linewidths, and optical spin pumping on single self-assembled InGaAs quantum dots embedded in a $162.5\,\text{nm}$ thin diode structure. The quantum dots are just $88\,\text{nm}$ from the top GaAs surface. We design and realize a p-i-n-i-n diode that allows single-electron charging of the quantum dots at close-to-zero applied bias. In operation, the current flow through the device is extremely small resulting in low noise. In resonance fluorescence, we measure optical linewidths below $2\,\mu\text{eV}$, just a factor of two above the transform limit. Clear optical spin pumping is observed in a magnetic field of $0.5\,\text{T}$ in the Faraday geometry. We present this design as ideal for securing the advantages of self-assembled quantum dots -- highly coherent single photon generation, ultra-fast optical spin manipulation -- in the thin diodes required in quantum nano-photonics and nano-phononics applications.

Emission wavelength selection for InGaAs quantum dots by anodic-aluminum-oxide membrane

Anodic-aluminum-oxide (AAO) membranes are fabricated and bonded on the surface of self-assembled InGaAs quantum dots (QDs) samples. The photoluminescence peak wavelengths for the AAO-bonded QDs samples are fixed despite by the different QDs structures of the samples, and the optical intensity is enhanced from the photonic-crystal radiation modes of the AAO quasi-periodic air-hole array.

Excitons and trions in single and vertically coupled quantum dots under an electric field

We present a theoretical study of the exciton (X0), the positive and negative trions (X+ and X−) in single and vertically coupled configurations of self-assembled InGaAs quantum dots under an electric field. The quantum states of X0, X+ and X− have been investigated using a quasi-one-dimensional (Q1D) model within the effective-mass approximation. For the single quantum dots, the electric-field dependent energy levels and the average inter-particle distances for the exciton and trions have been calculated. For the coupled quantum dots, the ground and the excited states for X0, X+ and X− have also been calculated and discussed. It is found that either the hole or the electron can be tuned into resonance states by the electric field and that the transition energy spectra for both trions consequently show crossing and anticrossing patterns. The recombination probabilities of the exciton and trion optical transitions are also calculated. The theoretical results have been compared with previously reported photoluminescence data and qualitative agreement is obtained. The trion conditional wave functions are also plotted under different electric field intensities, and it is found that a molecular orbital can be formed at a critical electric field intensity. The evolution of the energy levels of the trions in coupled quantum dots can be explained by the interplay of particle transfer and the electric field.

On-chip interference of single photons from an embedded quantum dot and an external laser

In this work, we demonstrate the on-chip two-photon interference between single photons emitted by a single self-assembled InGaAs quantum dot and an external laser. The quantum dot is embedded within one arm of an air-clad directional coupler which acts as a beam-splitter for incoming light. Photons originating from an attenuated external laser are coupled to the second arm of the beam-splitter and then combined with the quantum dot photons, giving rise to two-photon quantum interference between dissimilar sources. We verify the occurrence of on-chip Hong-Ou-Mandel interference by cross-correlating the optical signal from the separate output ports of the directional coupler. This experimental approach allows us to use a classical light source (laser) to assess in a single step the overall device performance in the quantum regime and probe quantum dot photon indistinguishability on application realistic time scales.

Dynamic vibronic coupling in InGaAs quantum dots [Invited

The electron-phonon coupling in self-assembled InGaAs quantum dots is relatively weak at low light intensities, which means that the zero-phonon line in emission is strong compared to the phonon sideband. However, the coupling to acoustic phonons can be dynamically enhanced in the presence of an intense optical pulse tuned within the phonon sideband. Recent experiments have shown that this dynamic vibronic coupling can enable population inversion to be achieved when pumping with a blue-shifted laser and for rapid de-excitation of an inverted state with red detuning. In this paper we confirm the incoherent nature of the phonon-assisted pumping process and explore the temperature dependence of the mechanism. We also show that a combination of blue- and red-shifted pulses can create and destroy an exciton within a timescale ~20 ps determined by the pulse duration and ultimately limited by the phonon thermalisation time.

Few-second-long correlation times in a quantum dot nuclear spin bath probed by frequency-comb nuclear magnetic resonance spectroscopy

One of the key challenges in spectroscopy is inhomogeneous broadening that masks the homogeneous spectral lineshape and the underlying coherent dynamics. A variety of techniques including four-wave mixing and spectral hole-burning are used in optical spectroscopy while in nuclear magnetic resonance (NMR) spin-echo is the most common way to counteract inhomogeneity. However, the high-power pulses used in spin-echo and other sequences often create spurious dynamics obscuring the subtle spin correlations that play a crucial role in quantum information applications. Here we develop NMR techniques that allow the correlation times of the fluctuations in a nuclear spin bath of individual quantum dots to be probed. This is achieved with the use of frequency comb excitation which allows the homogeneous NMR lineshapes to be measured avoiding high-power pulses. We find nuclear spin correlation times exceeding 1 s in self-assembled InGaAs quantum dots - four orders of magnitude longer than in strain-free III-V semiconductors. The observed freezing of the nuclear spin fluctuations opens the way for the design of quantum dot spin qubits with a well-understood, highly stable nuclear spin bath.

Emission redistribution from a quantum dot-bowtie nanoantenna

We present a combined experimental and simulation study of a single self-assembled InGaAs quantum dot coupled to a nearby ($\sim 25nm$) plasmonic antenna. Micro-photoluminescence spectroscopy shows a $\sim 2.4\times$ increase of intensity, which is attributed to spatial far-field redistribution of the emission from the quantum dot-antenna system. Power-dependent studies show similar saturation powers of $2.5\mu W$ for both coupled and uncoupled quantum dot emission in polarization-resolved measurements. Moreover, time-resolved spectroscopy reveals the absence of Purcell-enhancement of the quantum dot coupled to the antenna as compared to an uncoupled dot, yielding comparable exciton lifetimes of $\tau\sim0.5ns$. This observation is supported by numerical simulations, suggesting only minor Purcell-effects of $<2\times$ for emitter-antenna separations $>25nm$. The observed increased emission from a coupled quantum dot-plasmonic antenna system is found to be in good qualitative agreement with numerical simulations and will lead to a better understanding of light-matter-coupling in such novel semiconductor-plasmonic hybrid systems

On-Chip Generation, Routing, and Detection of Resonance Fluorescence.

Quantum optical circuits can be used to generate, manipulate, and exploit nonclassical states of light to push semiconductor based photonic information technologies to the quantum limit. Here, we report the on-chip generation of quantum light from individual, resonantly excited self-assembled InGaAs quantum dots, efficient routing over length scales ≥1 mm via GaAs ridge waveguides, and in situ detection using evanescently coupled integrated NbN superconducting single photon detectors fabricated on the same chip. By temporally filtering the time-resolved luminescence signal stemming from single quantum dots we use the quantum optical circuit to perform time-resolved excitation spectroscopy on single dots and demonstrate resonance fluorescence with a line-width of 10 ± 1 μeV; key elements needed for the use of single photons in prototypical quantum photonic circuits.

Dissipative preparation of the exciton and biexciton in self-assembled quantum dots on picosecond time scales

Pulsed resonant fluorescence is used to probe ultrafast phonon-assisted exciton and biexciton preparation in individual self-assembled InGaAs quantum dots. By driving the system using large area $(\ensuremath{\ge}10\ensuremath{\pi})$ near resonant optical pulses, we experimentally demonstrate how phonon-mediated dissipation within the manifold of dressed excitonic states can be used to prepare the neutral exciton with a fidelity $\ensuremath{\ge}70%$. By comparing the phonon-assisted preparation with resonant Rabi oscillations we show that the phonon-mediated process provides the higher-fidelity preparation for large pulse areas and is less sensitive to pulse area variations. Moreover, by detuning the laser with respect to the exciton transition, we map out the spectral density for exciton coupling to the bulk LA-phonon continuum. Similar phonon-mediated processes are shown to facilitate direct biexciton preparation via two-photon biexciton absorption, with fidelities $&gt;80%$. Our results are found to be in very good quantitative agreement with simulations that model the quantum dot--phonon bath interactions with Bloch-Redfield theory.

Annealing-induced change in quantum dot chain formation mechanism

Self-assembled InGaAs quantum dot chains were grown using a modified Stranski-Krastanov method in which the InGaAs layer is deposited under a low growth temperature and high arsenic overpressure, which suppresses the formation of dots until a later annealing process. The dots are capped with a 100 nm GaAs layer. Three samples, having three different annealing temperatures of 460°C, 480°C, and 500°C, were studied by transmission electron microscopy. Results indicate two distinct types of dot formation processes: dots in the 460°C and 480°C samples form from platelet precursors in a one-to-one ratio whereas the dots in the sample annealed at 500°C form through the strain-driven self-assembly process, and then grow larger via an additional Ostwald ripening process whereby dots grow into larger dots at the expense of smaller seed islands. There are consequently significant morphological differences between the two types of dots, which explain many of the previously-reported differences in optical properties. Moreover, we also report evidence of indium segregation within the dots, with little or no indium intermixing between the dots and the surrounding GaAs barrier.

Growth-temperature dependence of optical spin-injection dynamics in self-assembled InGaAs quantum dots

The growth-temperature dependence of the optical spin-injection dynamics in self-assembled quantum dots (QDs) of In0.5Ga0.5As was studied by increasing the sheet density of the dots from 2 × 1010 to 7 × 1010 cm−2 and reducing their size through a decrease in growth temperature from 500 to 470 °C. The circularly polarized transient photoluminescence (PL) of the resulting QD ensembles was analyzed after optical excitation of spin-polarized carriers in GaAs barriers by using rate equations that take into account spin-injection dynamics such as spin-injection time, spin relaxation during injection, spin-dependent state-filling, and subsequent spin relaxation. The excitation-power dependence of the transient circular polarization of PL in the QDs, which is sensitive to the state-filling effect, was also examined. It was found that a systematic increase occurs in the degree of circular polarization of PL with decreasing growth temperature, which reflects the transient polarization of exciton spin after spin injection. This is attributed to strong suppression of the filling effect for the majority-spin states as the dot-density of the QDs increases.

A carrier relaxation bottleneck probed in single InGaAs quantum dots using integrated superconducting single photon detectors

Using integrated superconducting single photon detectors, we probe ultra-slow exciton capture and relaxation dynamics in single self-assembled InGaAs quantum dots embedded in a GaAs ridge waveguide. Time-resolved luminescence measurements performed with on- and off-chip detection reveal a continuous decrease in the carrier relaxation time from 1.22 ± 0.07 ns to 0.10 ± 0.07 ns upon increasing the number of non-resonantly injected carriers. By comparing off-chip time-resolved spectroscopy with spectrally integrated on-chip measurements, we identify the observed dynamics in the rise time (τr) as arising from a relaxation bottleneck at low excitation levels. From the comparison with the temporal dynamics of the single exciton transition with the on-chip emission signal, we conclude that the relaxation bottleneck is circumvented by the presence of charge carriers occupying states in the bulk material and the two-dimensional wetting layer continuum. A characteristic τr ∝ P−2∕3 power law dependence is observed suggesting Auger-type scattering between carriers trapped in the quantum dot and the two-dimensional wetting layer continuum which circumvents the phonon relaxation bottleneck.