Single Quantum Dot Research Articles

Resonance-fluorescence spectral dynamics of an acoustically modulated quantum dot

Quantum technologies that rely on photonic qubits require a precise controllability of their properties. For this purpose hybrid approaches are particularly attractive because they offer a large flexibility to address different aspects of the photonic degrees of freedom. When combining photonics with other quantum platforms like phonons, quantum transducers have to be realized that convert between the mechanical and optical domain. Here, we realize this interface between phonons in the form of surface acoustic waves (SAWs) and single photons, mediated by a single semiconductor quantum dot exciton. In this combined theoretical and experimental study, we show that the different sidebands exhibit characteristic blinking dynamics that can be controlled by detuning the laser from the exciton transition. By developing analytical approximations we gain a better understanding of the involved internal dynamics. Our specific SAW approach allows us to reach the ideal frequency range of around 1 GHz that enables simultaneous temporal and spectral phonon sideband resolution close to the combined fundamental time-bandwidth limit.

Optically Driven Giant Superbunching from a Single Perovskite Quantum Dot

AbstractPhoton superbunching is a signature of a strong correlation between photons, which is a crucial resource needed in quantum communication and computation. As such, a superbunched photon source based on a material with high quantum efficiency, like cesium lead halide perovskite, is highly desirable. Utilizing the large dark–bright exciton splitting in CsPbBr3quantum dot (QD), the authors achieve a superbunching with a large g(2)(0) ≈ 30 from an optically driven single CsPbBr3QD emission at cryogenic temperature. The cascaded emission is identified as the cause of this superbunching by utilizing second‐order cross‐correlation measurement and exploring the excitation power and temperature dependence of the bunching level. The findings have immediate implications on the basic understanding of a single perovskite QD emission and its application as a quantum light source.

Metal, dielectric and hybrid nanoantennas for enhancing the emission of single quantum dots: A comparative study

The confinement of electromagnetic energy to subwavelength volumes through nanoscale antennas can be used to enhance the spontaneous emission of quantum emitters. With this aim, different configurations of metallic and high refractive index dielectric nanoparticles have been explored. Here, we carry out a comparative analysis of planar metallic, high refractive index dielectric, and hybrid nanoantennas considering three different parameters: the Purcell factor enhancement, radiation efficiency, and directionality properties. We focus our study on different geometries and material combinations of a dimer of cylinders. A dimer made of two gold nanocylinders is the most promising candidate for improving the spontaneous emission. While most previous works have paid attention to the redirection of the scattered emission in the nanoparticle plane, our proposed nanostructure of two large gold cylinders (R=λ/4) emits most of the radiation upwards. This effect is due to the strong quadrupolar electric contribution to the resonant mode. With the aim to further improve the directionality properties, additional silicon nanocylinders are used as directors of the scattered radiation, increasing the directivity by a factor of 2.4 with respect to the gold dimer without directors. All in all, a hybrid structure composed of a gold dimer and silicon nanoparticles is proposed to enhance the spontaneous emission of a single quantum dot and to govern its emission pattern. The results shown in this work could be useful in fluorescence enhancement or in quantum photonics. They are particularly interesting for the development of single-photon sources based on quantum dots and other nanoscale emitters.

Preparation and Readout of Multielectron High-Spin States in a Gate-Defined GaAs/AlGaAs Quantum Dot.

We report the preparation and readout of multielectron high-spin states, a three-electron quartet, and a four-electron quintet, in a gate-defined GaAs/AlGaAs single quantum dot using spin filtering by quantum Hall edge states coupled to the dot. The readout scheme consists of mapping from multielectron to two-electron spin states and a subsequent two-electron spin readout, thus obviating the need to resolve dense multielectron energy levels. Using this technique, we measure the relaxations of the high-spin states and find them to be an order of magnitude faster than those of low-spin states. Numerical calculations of spin relaxation rates using the exact diagonalization method agree with the experiment. The technique developed here offers a new tool for the study and application of high-spin states in quantum dots.

Heralded Spectroscopy Reveals Exciton-Exciton Correlations in Single Colloidal Quantum Dots.

Multiply excited states in semiconductor quantum dots feature intriguing physics and play a crucial role in nanocrystal-based technologies. While photoluminescence provides a natural probe to investigate these states, room-temperature single-particle spectroscopy of their emission has proved elusive due to the temporal and spectral overlap with emission from the singly excited and charged states. Here, we introduce biexciton heralded spectroscopy enabled by a single-photon avalanche diode array based spectrometer. This allows us to directly observe biexciton–exciton emission cascades and measure the biexciton binding energy of single quantum dots at room temperature, even though it is well below the scale of thermal broadening and spectral diffusion. Furthermore, we uncover correlations hitherto masked in ensembles of the biexciton binding energy with both charge-carrier confinement and fluctuations of the local electrostatic potential. Heralded spectroscopy has the potential of greatly extending our understanding of charge-carrier dynamics in multielectron systems and of parallelization of quantum optics protocols.

Single Photon Source from a Nanoantenna-Trapped Single Quantum Dot.

Single photon sources with high brightness and subnanosecond lifetimes are key components for quantum technologies. Optical nanoantennas can enhance the emission properties of single quantum emitters, but this approach requires accurate nanoscale positioning of the source at the plasmonic hotspot. Here, we use plasmonic nanoantennas to simultaneously trap single colloidal quantum dots and enhance their photoluminescence. The nano-optical trapping automatically locates the quantum emitter at the nanoantenna hotspot without further processing. Our dedicated nanoantenna design achieves a high trap stiffness of 0.6 (fN/nm)/mW for quantum dot trapping, together with a relatively low trapping power of 2 mW/μm2. The emission from the nanoantenna-trapped single quantum dot shows 7× increased brightness, 50× reduced blinking, 2× shortened lifetime, and a clear antibunching below 0.5 demonstrating true single photon emission. Combining nano-optical tweezers with plasmonic enhancement is a promising route for quantum technologies and spectroscopy of single nano-objects.

Quantum polyspectra for modeling and evaluating quantum transport measurements: A unifying approach to the strong and weak measurement regime

Quantum polyspectra of up to fourth order are introduced for modeling and evaluating quantum transport measurements offering a powerful alternative to methods of the traditional full counting statistics. Experimental time traces of the occupation dynamics of a single quantum dot are evaluated via simultaneously fitting their second-, third-, and fourth-order spectra. The scheme recovers the same electron tunneling and spin relaxation rates as previously obtained from an analysis of the same data in terms of factorial cumulants of the full counting statistics and waiting-time distributions. Moreover, the evaluation of time traces via quantum polyspectra is demonstrated to be feasible also in the weak measurement regime even when quantum jumps can no longer be identified from time traces and methods related to the full counting statistics cease to be applicable. A numerical study of a double dot system shows strongly changing features in the quantum polyspectra for the transition from the weak measurement regime to the Zeno regime where coherent tunneling dynamics is suppressed. Quantum polyspectra thus constitute a general unifying approach to the strong and weak regime of quantum measurements with possible applications in diverse fields as nanoelectronics, circuit quantum electrodynamics, spin noise spectroscopy, or quantum optics.

Enhanced Exciton Quantum Coherence in Single CsPbBr3 Perovskite Quantum Dots using Femtosecond Two-Photon Near-Field Scanning Optical Microscopy.

Cesium-halide perovskite quantum dots (QDs) have gained tremendous interest as quantum emitters in quantum information processing applications due to their optical and photophysical properties. However, engineering excitonic states in quantum dots requires a deep knowledge of the coherent dynamics of their excitons at a single-particle level. Here, we use femtosecond time-resolved two-photon near-field scanning optical microscopy (NSOM) to reveal coherences involving a single cesium lead bromide perovskite QD (CsPbBr3) at room temperature. We show that, compared to other nonperovskite nanoparticles, the electronic coherence on a single perovskite QD has a relatively long lifetime of ca. 150 fs, whereas CdSe QDs have exciton coherence times shorter than 75 fs at room temperature. One possible explanation for the longer coherence time observed for the CsPbBr3 perovskite system is related to the exciton fine structure of these perovskite QDs compared to other nanoparticles. These perovskite QDs exhibit interesting optical properties that differ from those of the traditional QDs including bright triplet exciton states. In fact, due to the small amplitude of the energy gap fluctuations of dipole-allowed triplet states in perovskite QDs, the coherent superposition could be preserved for longer times. Furthermore, single-particle excitation approach implemented in this work allows us to remove effects of heterogeneity that are usually present in ensemble averaging experiments at room temperature. The realization of quantum-mechanical phase-coherence of a charge carrier that can operate at room temperature is an issue of great importance for the potential application of coherent electronic phenomena in electronic and optoelectronic devices. These interesting findings provide further evidence of the great potential of these perovskite QDs as candidates for quantum computing and information processing applications.

Temporal shaping of single photons by engineering exciton dynamics in a single quantum dot

The majority of photonic quantum information technologies rely on single photons that have high purity and indistinguishability. Although solid-state quantum emitters can serve such single photons on demand, their asymmetric temporal and spatial mode profiles limit the optimal efficiency and fidelity of quantum interaction. Here, we demonstrate single-photon pulses at a telecom wavelength with a Gaussian-like temporal mode profile from a cavity-coupled single quantum dot. Engineering the exciton dynamics via multi-exciton cascade recombination and cavity detuning enables us to modify the rise and decay dynamics of single excitons. Furthermore, the cascade recombination process temporally retards the single-exciton emission from the background emission, leading to possible purification of single photons at high excitation power. In addition, coupling quantum dots into a low Q cavity mode leads to a Gaussian-like spatial mode profile, which brings a high collection efficiency. This approach paves the way for producing single photons with an optimized temporal and spatial waveform.

Membrane Nanoscopic Organization of D2L Dopamine Receptor Probed by Quantum Dot Tracking.

The role of lateral mobility and nanodomain organization of G protein-coupled receptors in modulating subcellular signaling has been under increasing scrutiny. Investigation of D2 dopamine receptor diffusion dynamics is of particular interest, as these receptors have been linked to altered neurotransmission in affective disorders and represent the primary target for commonly prescribed antipsychotics. Here, we applied our single quantum dot tracking approach to decipher intrinsic diffusion patterns of the wild-type long isoform of the D2 dopamine receptor and its genetic variants previously identified in several cohorts of schizophrenia patients. We identified a subtle decrease in the diffusion rate of the Val96Ala mutant that parallels its previously reported reduced affinity for potent neuroleptics clozapine and chlorpromazine. Slower Val96Ala variant diffusion was not accompanied by a change in receptor-receptor transient interactions as defined by the diffraction-limited quantum dot colocalization events. In addition, we implemented a Voronoї tessellation-based algorithm to compare nanoclustering of the D2 dopamine receptor to the dominant anionic phospholipid phosphatidylinositol 4,5-bisphosphate in the plasma membrane of live cells.

Crosstalk analysis for single-qubit and two-qubit gates in spin qubit arrays

Scaling up spin qubit systems requires high-fidelity single-qubit and two-qubit gates. Gate fidelities exceeding $98%$ were already demonstrated in silicon-based single and double quantum dots, whereas for the realization of larger qubit arrays, crosstalk effects on neighboring qubits must be taken into account. We analyze qubit fidelities impacted by crosstalk when performing single-qubit and two-qubit operations on neighbor qubits with a simple Heisenberg model. Furthermore, we propose conditions for driving fields to robustly synchronize Rabi oscillations and avoid crosstalk effects. In our analysis, we also consider crosstalk with two neighbors and show that double synchronization leads to a restricted choice for the driving field strength, exchange interaction, and thus gate time. Considering realistic experimental conditions, we propose a set of parameter values to perform a nearly crosstalk-free cnot gate and so open up the pathway to scalable quantum computing devices.

Photonic rocket structure grown by site-selective and bottom-up approach: A directional and Gaussian-like quantum emitter platform

Semiconductor quantum dots (QDs) integrated with photonic nanowires are one of the representative platforms for high-purity single photonic sources. However, conventional photonic nanowires suffer from severe scattering at the edge owing to the small footprint. For this reason, tapered structures have been adopted to achieve directional emission with minimized scattering, and hence, high light collection efficiency. So far, various tapered structures have been demonstrated by using top-down etching fabrication or catalyst-assisted growth. However, these approaches can induce critical issues for QD integrated photonic devices such as an etching damage, an inclusion of multiple QDs in a wire, a misalignment of QD with respect to the wire axis center, or a contamination of QD by the catalyst. Therefore, developing a catalyst-free, site-controlled growth technique is essential for high-quality tapered nanowire structures. In this work, we propose a site-selectively grown photonic rocket structure, which consists of a pencil-like nanowire and a pyramid acting as a single-mode waveguide and a coupler, respectively. Since this structure is defined by stable crystal facets, the dimensions of the structure, especially its tapering angle, are determined precisely. Most significantly, a single QD can be formed at the apex, deterministically aligned to the axis center of the photonic structure. We analyzed the propagating mode inside the photonic nanowire and pyramid coupler using finite-difference time-domain simulations. This photonic rocket structure produces directional emission owing to the pyramid coupler, resulting in 2.9 (2.0) times larger light collection efficiency with a numerical aperture of 0.3 (0.7), compared to the nanowire structure alone.

Nonequilibrium Kondo regime current noise spectrum of quantum dot systems with the single impurity Anderson model.

We investigate the nonequilibrium current noise spectrum of single impurity Anderson model quantum dot systems on the basis of the accurate dissipation equation of motion evaluations. By comparing between the equilibrium and nonequilibrium cases and between the non-Kondo and Kondo regimes, we identify the current noise spectrum of the nonequilibrium Kondo features that actually appear in the entire region of ω ∈ [-eV,eV]. It is well known that the primary Kondo characteristics at ω = ±eV = ±(μL -μR) display asymmetrical upturns and remarkable peaks in S(ω) and dS(ω)/dω, respectively. These features are originated from the Rabi interference of the transport current dynamics, with the Kondo oscillation frequency of |eV|. Moreover, we also identify the minor but very distinguishable inflections, crossing over from ω = -eV to ω = +eV. This uncovered feature would be related to the interference between two Kondo resonance channels.

Heat current rectification in a single quantum dot system with the presence and absence of the magnetic field

Heat current rectification in a single quantum dot system with the presence and absence of the magnetic field

Gate control, g factors, and spin-orbit energy of p -type GaSb nanowire quantum dot devices

Proposals for quantum information applications are frequently based on the coherent manipulation of spins confined to quantum dots. For these applications, p-type III-V material systems promise a reduction of the hyperfine interaction while maintaining large $g$-factors and strong spin-orbit interaction. In this work, we study bottom-gated device architectures to realize single and serial multi-quantum dot systems in Schottky contacted p-type GaSb nanowires. We find that the effect of potentials applied to gate electrodes on the nanowire is highly localized to the immediate vicinity of the gate electrode only, which prevents the formation of double quantum dots with commonly used device architectures. We further study the transport properties of a single quantum dot induced by bottom-gating, find large gate-voltage dependent variations of the $g^*$-factors up to $8.1\pm 0.2$ as well as spin-orbit energies between $110$-$230\,\mu$eV.

Adjustment of Terahertz Properties Assigned to the First Lowest Transition of (D+, X) Excitonic Complex in a Single Spherical Quantum Dot Using Temperature and Pressure

This theoretical study is devoted to the effects of pressure and temperature on the optoelectronic properties assigned to the first lowest transition of the (D+,X) excitonic complex (exciton-ionized donor) inside a single AlAs/GaAs/AlAs spherical quantum dot. Calculations are performed within the effective mass approximation theory using the variational method. Optical absorption and refractive index as function of the degree of confinement, pressure, and temperature are investigated. Numerical calculation shows that the pressure favors the electron-hole and electron-ionized donor attractions which leads to an enhancement of the binding energy, while an increasing of the temperature tends to reduce it. Our investigations show also that the resonant peaks of the absorption coefficient and the refractive index are located in the terahertz region and they undergo a shift to higher (lower) therahertz frequencies when the pressure (temperature) increases. The opposite effects caused by temperature and pressure have great practical importance because they offer an alternative approach for the adjustment and the control of the optical frequencies resulting from the transition between the fundamental and the first excited state of exciton bound to an ionized dopant. The comparison of the optical properties of exciton, impurity and (D+,X) facilitates the experimental identification of these transitions which are often close. Our investigation shows that the optical responses of (D+,X) are located between the exciton (high energy region) and donor impurity (low energy region) peaks. The whole of these conclusions may lead to the novel light detector or source of terahertz range.

Single quantum emitters detection with amateur CCD: Comparison to a scientific-grade camera

Fluorescence imaging of single quantum light emitters (atoms, molecules, quantum dots, color centers in crystals) is an inherent experimental problem of modern photonics and its numerous applications. In these measurements, highly sensitive cameras are of the key significance. Recent progress in technologies of charge-coupling devices (CCD) and complementary metal-oxide semiconductor (CMOS) sensors opens up possibilities for detection of extreme low light signals up to a single photon counting. Here, we investigate the parameters of high-professional scientific- and amateur-grade cameras in the view of their use in the fluorescence nanoscopy with the detection of single molecules and, in general, quantum emitters of different nature. A series of photoluminescence imaging experiments have been conducted with single colloidal semiconductor core-shell nanocrystals CdSeS/ZnS (quantum dots, QD), which are usually considered as a basis of various sensors and actuators technologies. We find parameters of the experiment for the amateur-grade camera to obtain images of single QDs with signal-to-noise ratio compared to the scientific-grade camera at exposure times ranging from 1s to 1000s.

Biexciton Binding Energy and Line width of Single Quantum Dots at Room Temperature.

Broadening of multiexciton emission from colloidal quantum dots (QDs) at room temperature is important for their use in high-power applications, but an in-depth characterization has not been possible until now. We present and apply a novel spectroscopic method to quantify the biexciton line width and biexciton binding energy of single CdSe/CdS/ZnS colloidal QDs at room temperature. In our method, which we term “cascade spectroscopy”, we select emission events from the biexciton cascade and reconstruct their spectrum. The biexciton has an average emission line width of 86 meV on the single-QD scale, similar to that of the exciton. Variations in the biexciton repulsion (Eb = 4.0 ± 3.1 meV; mean ± standard deviation of 15 QDs) are correlated with but are more narrowly distributed than variations in the exciton energy (10.0 meV standard deviation). Using a simple quantum-mechanical model, we conclude that inhomogeneous broadening in our sample is primarily due to variations in the CdS shell thickness.

InP-based single-photon sources operating at telecom C-band with increased extraction efficiency

In this work, we demonstrate a triggered single-photon source operating at the telecom C-band with photon extraction efficiency exceeding any reported values in this range. The non-classical light emission with low probability of the multiphoton events is realized with single InAs quantum dots (QDs) grown by molecular beam epitaxy and embedded directly in an InP matrix. Low QD spatial density on the order of 5 × 108 cm−2 to ∼2 × 109 cm−2 and symmetric shape of these nanostructures together with spectral range of emission make them relevant for quantum communication applications. The engineering of extraction efficiency is realized by combining a bottom distributed Bragg reflector consisting of 25 pairs of InP/In0.53Ga0.37Al0.1 As layers and cylindrical photonic confinement structures. Realization of such a technologically non-demanding approach even in a non-deterministic fashion results in photon extraction efficiency of (13.3 ± 2) % into 0.4 numerical aperture detection optics at approximately 1560 nm emission wavelength, i.e., close to the center of the telecom C-band.

Optical feedback-induced dynamics and nonclassical photon statistics of semiconductor microcavity laser

We study a coherently driven semiconductor laser cavity containing a single quantum dot(QD) (as gain medium) with optical feedback under Markovian approximation. We have obtained coupled operator equations for the model Hamiltonian using standard input-output formalism of cavity-QED and have found that these equations do not have any finite steady state solutions. We have also used an exact numerical framework based on Matlab platform qotoolbox, to compute the temporal dynamics of the mean excitation number of laser cavity mode under high feedback coupling regime. We have further studied the photon correlations of both the cavity mode as well as external feedback mode to feedback identify the laser parameters and coupling strength that give the nonclassical sub-Poissonian photon statistics. This work is useful for coherent control of photon statistics and photon correlations in the semiconductor laser with optical feedback.