Realistic Quantum Dot Research Articles

Classical Force Field Parameters for InP and InAs Quantum Dots with Various Surface Passivations.

Classical molecular dynamics (MD) simulations on realistic colloidal quantum dot (QD) systems are often hampered by missing force field (FF) parameters for an accurate description of the QD-ligand interface. However, such calculations are of major interest, specifically for studying the surface chemistry of colloidal nanocrystals. In this work, we have utilized a previously published stochastic optimization algorithm to obtain FF parameters for InP and InAs QDs capped by Cl, amine, carboxylate, and thiolate ligands. Our FF parameters are interfaced with well-established FFs for organic molecules, allowing for the simulation of InP and InAs QDs with a broad range of organic ligands in explicit apolar solvents. The quality of our FF parameters was assessed by comparing properties of the classical MD simulations with ab initio MD simulations and experimental and theoretical values from the literature.

Noise-resistant quantum memory enabled by Hamiltonian engineering

Nuclear spins in quantum dots are promising candidates for fast and scalable quantum memory. By utilizing the hyperfine interaction between the central electron and its surrounding nuclei, quantum information can be transferred to the collective state of the nuclei and be stored for a long time. However, nuclear spin fluctuations in a partially polarized nuclear bath deteriorate the quantum memory fidelity. Here we introduce a noise-resistant protocol to realize fast and high-fidelity quantum memory through Hamiltonian engineering. With analytics and numerics, we show that high-fidelity quantum state transfer between the electron and the nuclear spins is achievable at relatively low nuclear polarizations, due to the strong suppression of nuclear spin noises. For a realistic quantum dot with $10^4$ nuclear spins, a fidelity surpassing 80% is possible at a polarization as low as 30%. Our approach reduces the demand for high nuclear polarization, making experimentally realizing quantum memory in quantum dots more feasible.

Using the Autler-Townes and ac Stark effects to optically tune the frequency of indistinguishable single photons from an on-demand source

We describe how a coherent optical drive that is near resonant with the upper rungs of a three-level ladder system, in conjunction with a short-pulse excitation, can be used to provide a frequency-tunable source of on-demand single photons. Using an intuitive master equation model, we identify two distinct regimes of device operation: (i) for a resonant drive, the source operates using the Autler-Townes effect, and (ii) for an off-resonant drive, the source exploits the ac Stark effect. The former regime allows for a large frequency-tuning range but coherence suffers from timing jitter effects, while the latter allows for high indistinguishability and efficiency, but with a restricted tuning bandwidth due to high required drive strengths and detunings. We show how both these negative effects can be mitigated by using an optical cavity to increase the collection rate of the desired photons. We apply our general theory to semiconductor quantum dots, which have proven to be excellent single-photon sources, and find that scattering of acoustic phonons leads to excitation-induced dephasing and increased population of the higher-energy level which limits the bandwidth of frequency tuning achievable while retaining high indistinguishability. Despite this, for realistic cavity and quantum dot parameters, indistinguishabilities of over $90%$ are achievable for energy shifts of up to hundreds of $\ensuremath{\mu}\mathrm{eV}$, and near-unity indistinguishabilities for energy shifts up to tens of $\ensuremath{\mu}\mathrm{eV}$. Additionally, we clarify the often-overlooked differences between an idealized Hong-Ou-Mandel two-photon interference experiment and its usual implementation with an unbalanced Mach-Zehnder interferometer, pointing out the subtle differences in the single-photon visibility associated with these different setups.

Negligible contribution of inter-dot coherent modes to heat conduction in quantum-dot superlattice

Colloidal quantum dots (QDs) superlattice, which is made of inorganic cores and can self-assemble into various types of lattice structures, finds promising applications in optical, electrical, and optoelectronic devices. Recent inelastic neutron scattering measurement [NAT. COMMUN. 10:4236 (2019)] showed that the inter-quantum-dot vibrational frequencies can be tuned by varying the QDs shapes and ligand types, suggesting that the QDs superlattices can be a platform for phonon engineering. In this work, we quantify the impact of the second periodicity on thermal transport through full-scale molecular dynamics simulations of PbS QDs superlattice with realistic QD size and ligand morphology. The vibrational pattern analysis reveals that the vibrations can be classified into the inter-QDs coherent modes and the spatially localized modes arising from the geometry confinement. The spectral analysis indicates that spatially localized modes in the frequency range of 0.8–5 THz dominate the thermal transport and lead to an amorphous-like temperature dependence between 200 and 400 K. On the other hand, the inter-QDs coherent modes, albeit have an averaged relaxation of 10 ps, have a limited thermal conductivity value of 0.01 W/mK at room temperature due to the scarce of the vibrational states. We demonstrate that controlling the ligand morphology is more efficient than tuning the second periodicity in engineering the thermal conductivity of QDs superlattice.

Evaluation of synthetic and experimental training data in supervised machine learning applied to charge-state detection of quantum dots

Automated tuning of gate-defined quantum dots is a requirement for large-scale semiconductor-based qubit initialisation. An essential step of these tuning procedures is charge-state detection based on charge stability diagrams. Using supervised machine learning to perform this task requires a large dataset for models to train on. In order to avoid hand labelling experimental data, synthetic data has been explored as an alternative. While providing a significant increase in the size of the training dataset compared to using experimental data, using synthetic data means that classifiers are trained on data sourced from a different distribution than the experimental data that is part of the tuning process. Here we evaluate the prediction accuracy of a range of machine learning models trained on simulated and experimental data, and their ability to generalise to experimental charge stability diagrams in two-dimensional electron gas and nanowire devices. We find that classifiers perform best on either purely experimental or a combination of synthetic and experimental training data, and that adding common experimental noise signatures to the synthetic data does not dramatically improve the classification accuracy. These results suggest that experimental training data as well as realistic quantum dot simulations and noise models are essential in charge-state detection using supervised machine learning.

GANDA: A deep generative adversarial network conditionally generates intratumoral nanoparticles distribution pixels-to-pixels

Intratumoral nanoparticles (NPs) distribution is critical for the success of nanomedicine in imaging and treatment, but computational models to describe the NPs distribution remain unavailable due to the complex tumor-nano interactions. Here, we develop a Generative Adversarial Network for Distribution Analysis (GANDA) to describe and conditionally generates the intratumoral quantum dots (QDs) distribution after i.v. injection. This deep generative model is trained automatically by 27,775 patches of tumor vessels and cell nuclei decomposed from whole-slide images of 4 T1 breast cancer sections. The GANDA model can conditionally generate images of intratumoral QDs distribution under the constraint of given tumor vessels and cell nuclei channels with the same spatial resolution (pixels-to-pixels), minimal loss (mean squared error, MSE = 1.871) and excellent reliability (intraclass correlation, ICC = 0.94). Quantitative analysis of QDs extravasation distance (ICC = 0.95) and subarea distribution (ICC = 0.99) is allowed on the generated images without knowing the real QDs distribution. We believe this deep generative model may provide opportunities to investigate how influencing factors affect NPs distribution in individual tumors and guide nanomedicine optimization for molecular imaging and personalized treatment.

Efficient electronic structure calculations for extended systems of coupled quantum dots using a linear combination of quantum dot orbitals method

We present a novel "linear combination of atomic orbitals"-type of approximation, enabling accurate electronic structure calculations for systems of up to 20 or more electronically coupled quantum dots. Using realistic single quantum dot wavefunctions as basis to expand the eigenstates of the heterostructure, our method shows excellent agreement with full 8-band $\boldsymbol{k}\cdot\boldsymbol{p}$ calculations, exemplarily chosen for our benchmarking comparison, with an orders of magnitude reduction in computational time. We show that, in order to correctly predict the electronic properties of such stacks of coupled quantum dots, it is necessary to consider the strain distribution in the whole heterostructure. Edge effects determine the electronic structure for stacks of $\lesssim$ 10 QDs, after which a homogeneous confinement region develops in the center. The overarching goal of our investigations is to design a stack of vertically coupled quantum dots with an intra-band staircase potential suitable as active material for a quantum-dot-based quantum cascade laser. Following a parameter study in the In$_{x}$Ga$_{1-x}$As/GaAs material system, varying quantum dot size, material composition and inter-dot coupling strength, we show that an intra-band staircase potential of identical transitions can in principle be realized. A species library we generated for over 800 unique quantum dots provides easy access to the basis functions required for different realizations of heterostructures. In the associated manuscript entitled "Room Temperature Lasing of Terahertz Quantum Cascade Lasers Based on a Quantum Dot Superlattice", we investigate room temperature lasing of a terahertz quantum cascade laser based on a two-quantum-dot unit cell superlattice.

Modelling and simulation of carrier transport in quantum dot memory device for longer data retention and minimized power consumption

The performance of a group III–V material quantum dot (QD) nanostructure memory is investigated using a self-consistent Schrodinger solver, eight-band k·p model, and carrier dynamics modelling. This model is used to explore the information loss due to the carrier emission rate in the QDs as a function of temperature, size and confinement potential. The results reveal the dominant emission mechanisms that should occur at different operating temperatures. To minimize the loss and improve the performance at room temperature, our findings reveal an increase in the carrier storage time and a reduction in the power dissipation with increasing dot size. It is further illustrated that electrons are advantageous as information carriers over holes and that the inclusion of high-bandgap barrier layers favours longer-duration data retention. The model is extended to include trap states in realistic QDs, whose effect is found to become more prominent with performance optimization. The computed results are in close agreement with other experimental data for different QDs along with barrier layer. This validates the efficacy of the model, which can be utilized as a design tool for fabricating nanoscale memories with better data retention capability.

Collective ground states in small lattices of coupled quantum dots

Motivated by recent developments on the fabrication and control of semiconductor-based quantum dot qubits, we theoretically study a finite system of tunnel-coupled quantum dots with the electrons interacting through the long-range Coulomb interaction. When the inter-electron separation is large and the quantum dot confinement potential is weak, the system behaves as an effective Wigner crystal with a period determined by the electron average density with considerable electron hopping throughout the system. For stronger periodic confinement potentials, however, the system makes a crossover to a Mott-type strongly correlated ground state where the electrons are completely localized at the individual dots with little inter-dot tunneling. In between these two phases, the system is essentially a strongly correlated electron liquid with inter-site electron hopping constrained by strong Coulomb interaction. We characterize this Wigner-Mott-liquid quantum crossover with detailed numerical finite-size diagonalization calculations of the coupled interacting qubit system, showing that these phases can be smoothly connected by tuning the system parameters. Experimental feasibility of observing such a hopping-tuned Wigner-Mott-liquid crossover in currently available semiconductor quantum dot qubits is discussed. In particular, we connect our theoretical results to recent quantum-dot-based quantum emulation experiments where collective Coulomb blockade was demonstrated. One conclusion of our theory is that currently available realistic quantum dot arrays are unable to explore the low-density Wigner phase with only the Mott-liquid crossover being accessible experimentally.

Discrete time crystal in the gradient-field Heisenberg model

We show that time crystal phases, which are known to exist for disorder-based many-body localized systems, also appear in systems where localization is due to strong magnetic field gradients. Specifically, we study a finite Heisenberg spin chain in the presence of a gradient field, which can be realized experimentally in quantum dot systems using micromagnets or nuclear spin polarization. Our numerical simulations reveal time crystalline order over a broad range of realistic quantum dot parameters, as evidenced by the long-time preservation of spin expectation values and the asymptotic form of the mutual information. We also consider the undriven system and present several diagnostics for many-body localization that are complementary to those recently studied. Our results show that these non-ergodic phases should be realizable in modest-sized quantum dot spin arrays using only demonstrated experimental capabilities.

Inhomogeneous Broadening of the Exciton Band in Optical Absorption Spectra of InP/ZnS Nanocrystals.

In this work, we have simulated the processes of broadening the first exciton band in optical absorption spectra (OA) for InP/ZnS ensembles of colloidal quantum dots (QDs). A phenomenological model has been proposed that takes into account the effects of the exciton–phonon interaction, and allows one to analyze the influence of the static and dynamic types of atomic disorder on the temperature changes in the spectral characteristics in question. To vary the degree of static disorder in the model system, we have used a parameter δ, which characterizes the QD dispersion in size over the ensemble. We have also calculated the temperature shifts of the maxima and changes in the half-width for the exciton peaks in single nanocrystals (δ = 0), as well as for the integrated OA bands in the QD ensembles with different values of δ = 0.6–17%. The simulation results and the OA spectra data measured for InP/ZnS nanocrystals of 2.1 nm (δ = 11.1%) and 2.3 nm (δ = 17.3%), are in good mutual agreement in the temperature range of 6.5 K–RT. It has been shown that the contribution of static disorder to the observed inhomogeneous broadening of the OA bands for the QDs at room temperature exceeds 90%. The computational experiments performed indicate that the temperature shift of the maximum for the integrated OA band coincides with that for the exciton peak in a single nanocrystal. In this case, a reliable estimate of the parameters of the fundamental exciton–phonon interaction can be made. Simultaneously, the values of the specified parameters, calculated from the temperature broadening of the OA spectra, can be significantly different from the true ones due to the effects of static atomic disorder in real QD ensembles.

Effects of electrostatic environment on the electrically triggered production of entangled photon pairs from droplet epitaxial quantum dots

Entangled photon pair generation is a crucial task for development of quantum information based technologies, and production of entangled pairs by biexciton cascade decays in semiconductor quantum dots is so far one of the most advanced techniques to achieve it. However, its scalability toward massive implementation requires further understanding and better tuning mechanisms to suppress the fine structure splitting between polarized exciton states, which persists as a major obstacle for entanglement generation from most quantum dot samples. In this work, the influence of electrostatic environment arising from electrically biased electrodes and/or charged impurities on the fine structure splitting of GaAs/AlGaAs droplet epitaxial quantum dots is studied, by means of numerical simulations considering a realistic quantum dot confining potential and electron-hole exchange interaction within a multiband k · p framework. We find that reduction of the fine structure splitting can be substantially optimized by tilting the field and seeding impurities along the droplet elongation axis. Furthermore, our results provide evidence of how the presence of charged impurities and in-plane bias components, may account for different degrees of splitting manipulation in dots with similar shape, size and growth conditions.

Electronic Structure Origins of Surface-Dependent Growth in III–V Quantum Dots

Indium phosphide quantum dots (QDs) have emerged as a promising candidate to replace more toxic II–VI CdSe QDs, but production of high-quality III–V InP QDs with targeted properties requires a better understanding of their growth. We develop a first-principles-derived model that unifies InP QD formation from isolated precursor and early stage cluster reactions to 1.3 nm magic sized clusters and rationalize experimentally observed properties of full sized >3 nm QDs. Our first-principles study on realistic QD models reveals large surface-dependent reactivity for all elementary growth process steps, including In-ligand bond cleavage and P precursor addition. These thermodynamic trends correlate well to kinetic properties at all stages of growth, indicating the presence of labile and stable spots on cluster and QD surfaces. Correlation of electronic or geometric properties to energetics identifies surprising sources for these variations: short In···In separation on the surface produces the most reactive sites, at odds with conventional understanding of strain (i.e., separation) in bulk metallic surfaces increasing reactivity and models for ionic II–VI QD growth. These differences are rationalized by the covalent, directional nature of bonding in III–V QDs and explained by bond order metrics derived directly from the In–O bond density. The unique constraints of carboxylate and P precursor bonding to In atoms rationalize why all sizes of InP clusters and QDs are In-rich but become less so as QDs mature. These observations support the development of alternate growth recipes that take into account strong surface-dependence of kinetics as well as the shapes of both In and P precursors to control both kinetics and surface morphology in III–V QDs.

Force field potentials for the vibrational properties of II-VI semiconductor nanostructures

We derive force field potentials for CdS, CdSe, CdTe, ZnS, ZnSe, and ZnTe using the vibrational and elastic properties of the bulk materials based on density functional theory calculations and experiment. The potentials have bond-stretching (first- and second-nearest neighbor), bond-bending, as well as long-range Coulomb interactions. The bulk vibrational properties are very well reproduced for all materials considered. The vibrational properties of nanoclusters are compared to the results of large-scale density functional theory calculations with up to 1000 atoms. We obtain a very good agreement for all the core vibrational modes and an overall reasonable agreement over the entire spectrum. However, the low-frequency acoustic-type modes with surface character tend to be too soft in the force field calculations. We demonstrate the capability of the force field to obtain vibrational properties of realistic colloidal quantum dots with sizes up to 60 \AA{} diameter.

LIGHT ABSORPTION of SMALL CdS QUANTUM DOTS

The aim of article is to analyze the conditions of the interface states arise which caused by the polarization trap, and determine the impact of these conditions on the light absorption. Therefore, it was determined the energy of interface states caused by polarization charges arising on heteroboundaries. For calculations we took into account two models: the transition layer on the interface and his absence. In both cases, we shown that polarization traps exist, which can capture the electrons in the case of the small size of quantum dots. The energy spectrum of surface states was calculated by the Ritz variational method. A comparison of these energy states with energy internal states was made.The internal states are defined accurately using the effective masses approximation and the model of rectangular potential wells and barriers. This made it possible to conclude that for the real quantum dot size, the ground state of an electron is always in the internal states of quantum dot. Excited state is not affected. The dependence of the surface states energy on the quantum dot size was obtained. The corresponding energy of these states increases with decreasing of the quantum dot size. This is due to the polarization dependence of the depth of the trap sizes.We calculated matrix elements of the dipole moment of interlrvel transitions into surface states. The light absorption coefficient caused by the interlrvel transitions was defined as a function of the electromagnetic wave frequency. In the final formula of absorption coefficient, we take into account the quantum dots size distribution. It is shown that absorption bands which corresponds to electron transitions into surface states is much smaller than the absorption bands caused by transitions between inner states.

Atomistic theory of excitonic fine structure in InAs/InP nanowire quantum dot molecules

Nanowire quantum dots have peculiar electronic and optical properties. In this work we use atomistic tight binding to study excitonic spectra of artificial molecules formed by a double nanowire quantum dot. We demonstrate a key role of atomistic symmetry and nanowire substrate orientation rather than cylindrical shape symmetry of a nanowire and a molecule. In particular for $[001]$ nanowire orientation we observe a nonvanishing bright exciton splitting for a quasimolecule formed by two cylindrical quantum dots of different heights. This effect is due to interdot coupling that effectively reduces the overall symmetry, whereas single uncoupled $[001]$ quantum dots have zero fine structure splitting. We found that the same double quantum dot system grown on $[111]$ nanowire reveals no excitonic fine structure for all considered quantum dot distances and individual quantum dot heights. Further we demonstrate a pronounced, by several orders of magnitude, increase of the dark exciton optical activity in a quantum dot molecule as compared to a single quantum dot. For $[111]$ systems we also show spontaneous localization of single particle states in one of nominally identical quantum dots forming a molecule, which is mediated by strain and origins from the lack of the vertical inversion symmetry in $[111]$ nanostructures of overall ${C}_{3v}$ symmetry. Finally, we study lowering of symmetry due to alloy randomness that triggers nonzero excitonic fine structure and the dark exciton optical activity in realistic nanowire quantum dot molecules of intermixed composition.

Impact of Phonons on Dephasing of Individual Excitons in Deterministic Quantum Dot Microlenses.

Optimized light–matter coupling in semiconductor nanostructures is a key to understand their optical properties and can be enabled by advanced fabrication techniques. Using in situ electron beam lithography combined with a low-temperature cathodoluminescence imaging, we deterministically fabricate microlenses above selected InAs quantum dots (QDs), achieving their efficient coupling to the external light field. This enables performing four-wave mixing microspectroscopy of single QD excitons, revealing the exciton population and coherence dynamics. We infer the temperature dependence of the dephasing in order to address the impact of phonons on the decoherence of confined excitons. The loss of the coherence over the first picoseconds is associated with the emission of a phonon wave packet, also governing the phonon background in photoluminescence (PL) spectra. Using theory based on the independent boson model, we consistently explain the initial coherence decay, the zero-phonon line fraction, and the line shape of the phonon-assisted PL using realistic quantum dot geometries.

Broadband light sources based on InAs/InGaAs metamorphic quantum dots

We propose a design for a semiconductor structure emitting broadband light in the infrared, based on InAs quantum dots (QDs) embedded into a metamorphic step-graded InxGa1−xAs buffer. We developed a model to calculate the metamorphic QD energy levels based on the realistic QD parameters and on the strain-dependent material properties; we validated the results of simulations by comparison with the experimental values. On this basis, we designed a p-i-n heterostructure with a graded index profile toward the realization of an electrically pumped guided wave device. This has been done by adding layers where QDs are embedded in InxAlyGa1−x−yAs layers, to obtain a symmetric structure from a band profile point of view. To assess the room temperature electro-luminescence emission spectrum under realistic electrical injection conditions, we performed device-level simulations based on a coupled drift-diffusion and QD rate equation model. On the basis of the device simulation results, we conclude that the present proposal is a viable option to realize broadband light-emitting devices.

Coulomb Mediated Hybridization of Excitons in Coupled Quantum Dots.

We report Coulomb mediated hybridization of excitonic states in optically active InGaAs quantum dot molecules. By probing the optical response of an individual quantum dot molecule as a function of the static electric field applied along the molecular axis, we observe unexpected avoided level crossings that do not arise from the dominant single-particle tunnel coupling. We identify a new few-particle coupling mechanism stemming from Coulomb interactions between different neutral exciton states. Such Coulomb resonances hybridize the exciton wave function over four different electron and hole single-particle orbitals. Comparisons of experimental observations with microscopic eight-band k·p calculations taking into account a realistic quantum dot geometry show good agreement and reveal that the Coulomb resonances arise from broken symmetry in the artificial semiconductor molecule.

Ballistic to diffusive transition in a two-dimensional quantum dot lattice

Two-dimensional networks of ordered quantum dots beyond the percolation threshold are studied, as typical example of conducting nanostructures with quenched random disorder. Theory predicts anomalous diffusion with stretched-exponential relaxation at short distances, and computer simulations on lattices of crossing, straight paths of random length confirm such a behavior. Anomalous diffusion is interpreted as resulting from the higher probability of taking straight, or ballistic paths, when the traveled distance is comparable or shorter than the lattice characteristic length. Diffusion turns over to normal for longer traveled distances, whence all paths tend to become equiprobable. Such random lattice structures represent a model for realistic quantum dot networks, with potential applications in optoelectronics, photovoltaics or spintronics.