Single Quantum Dot Research Articles

CNOT Quantum Gate Based on Spatial Photonic Qubits Under Resonant Electro-Optical Control

A theoretical model of a quantum node that implements the two-qubit CNOT operation with use of photonic qubits with spatial encoding is considered. Each qubit is represented by a pair of modes supporting an arbitrary superposition of single-photon states. The active element of the node is a single or double quantum dot with a tunable frequency, which coherently exchanges an energy quantum with the modes. The spectral characteristics of the quantum node elements are simulated. The probability of implementation of a controlled inversion of the qubit state is calculated depending on the system parameters.

Heralded Generation of Correlated Photon Pairs from CdS/CdSe/CdS Quantum Shells.

Quantum information processing demands efficient quantum light sources (QLS) capable of producing high-fidelity single photons or entangled photon pairs. Single epitaxial quantum dots (QDs) have long been proven to be efficient sources of deterministic single photons; however, their production via molecular-beam epitaxy presents scalability challenges. Conversely, colloidal semiconductor QDs offer scalable solution processing and tunable photoluminescence, but suffer from broader linewidths and unstable emissions. This leads to spectrally inseparable emission from exciton (X) and biexciton (XX) states, complicating the production of single photons and triggered photon pairs. Here, we demonstrate that colloidal semiconductor quantum shells (QSs) achieve significant spectral separation (∼75-80 meV) and long temporal stability of X and XX emissive states, enabling the observation of exciton-biexciton bunching in colloidal QDs. Our low-temperature single-particle measurements show cascaded XX-X emission of single photon pairs for over 200 s, with minimal overlap between X and XX features. The X-XX distinguishability allows for an in-depth theoretical characterization of cross-correlation strength, placing it in perspective with photon pairs of epitaxial counterparts. These findings highlight a strong potential of semiconductor quantum shells for applications in quantum information processing.

Determination of the particle size distribution of cube-shaped colloidal perovskite quantum dots from photoluminescence spectra: A combined theoretical-experimental approach.

A theoretical-experimental approach is proposed to convert the photoluminescence spectra of colloidal perovskite quantum dot ensembles into accurate estimates for their intrinsic particle size distribution functions. Two main problems were addressed and properly correlated: the size dependence of the first excitonic transition in a single cube-shaped quantum dot and the inhomogeneous broadening of the fluorescence line shape due to the size nonuniformity of the chemically prepared quantum dot suspension in addition to the single-dot homogeneous broadening. By applying the reported methodology to CsPbBr3 quantum dot samples belonging to the strong and intermediate confinement regimes, the calculated size distributions exhibited close agreement with those obtained from transmission electron microscopy, with precise estimates for the average particle size and standard deviation. Specifically for strongly confined ultrasmall CsPbBr3 quantum dots, the presented spectroscopic model for size distribution computation is based on a new analytical expression for the size-dependent bandgap, which was developed within the framework of the finite-depth square-well effective mass approximation accounting for band nonparabolicity effects. Such a quantum mechanical approach correctly predicts the expected transition to the intermediate confinement regime in sufficiently large quantum dots, which are traditionally described by the well-known bandgap equation in the infinite potential barrier limit with a spatially correlated electron-hole wavefunction and nonparabolic carrier effective masses. The proposed calculation scheme originates from general theoretical considerations so that it can be readily adapted to semiconductor quantum dots of many other systems, from all inorganic metal halides to hybrid perovskite materials, regardless of the adopted chemical synthesis route.

Robust quantum dots charge autotuning using neural network uncertainty

Abstract This study presents a machine-learning-based procedure to automate the charge tuning of semiconductor spin qubits with minimal human intervention, addressing one of the significant challenges in scaling up quantum dot technologies. This method exploits artificial neural networks to identify noisy transition lines in stability diagrams, guiding a robust exploration strategy leveraging neural networks' uncertainty estimations. Tested across three distinct offline experimental datasets representing different single quantum dot technologies, the approach achieves over 99% tuning success rate in optimal cases, where more than 10% of the success is directly attributable to uncertainty exploitation. The challenging constraints of small training sets containing high diagram-to-diagram variability allowed us to evaluate the capabilities and limits of the proposed procedure.


High-dimensional quantum key distribution using orbital angular momentum of single photons from a colloidal quantum dot at room temperature

High-dimensional quantum key distribution (HDQKD) is a promising avenue to address the inherent limitations of basic quantum key distribution (QKD) protocols. However, experimental realizations of HDQKD to date have relied on indeterministic photon sources that limit the achievable key rate. In this paper, we demonstrate a full emulation of a HDQKD system using a single colloidal giant quantum dot (gQD) as a deterministic, compact, and room-temperature single-photon source (SPS). We demonstrate a practical protocol by encoding information in a high-dimensional space (d = 3) of the orbital angular momentum of the photons. Our experimental configuration incorporates two spatial light modulators for encoding and decoding the spatial information carried by individual photons. Our experimental demonstration establishes the feasibility of utilizing high radiative quantum yield gQDs as practical SPSs for HDQKD. We also experimentally demonstrate surpassing the traditional d = 2 QKD capacity with comparable error rates, indicating a significant improvement in performance while maintaining reliability.

Design of the Single Heterogeneous Quantum Dot Lasers Emitting 4 Wavelengths Using Combination‐Grating Technology

AbstractMulti‐wavelength light sources are crucial for high‐bandwidth silicon photonic chips. In this paper, a single heterogeneous quantum dot distributed feedback (DFB) laser emitting 4 wavelengths using the combination‐grating technology is designed. To the best of the knowledge, this is the first heterogeneously integrated quantum dot DFB laser that lases stable multi‐wavelength in a single cavity. When the etching depth, etching width, and total length of gratings are 100 , 550 nm, and 1 000 µm, respectively, 4‐wavelength with 1297.01 , 1303.38 , 1309.74 , and 1316.11 nm are obtained by varying the grating period from 196 to 199 nm with the spacing of 1 nm. Compared to the conventional DFB laser arrays, the DFB laser units are significantly reduced by 3/4 while maintaining the same number of output wavelengths. Additionally, by optimizing the λ/4 phase‐shift position and the duty cycle of gratings, the output power at the front‐end of the 4‐wavelength laser is significantly improved. Specifically, the ratio of the output power from the front‐end and rear‐end of the laser increases from the conventional 1.00 to 2.51. This work provides a competitive candidate for multi‐wavelength, high‐performance, and large‐scale silicon‐based light sources used in data centers, lidar, and component detection.

Scalable on-chip multiplexing of silicon single and double quantum dots

Owing to the maturity of complementary metal oxide semiconductor (CMOS) microelectronics, qubits realized with spins in silicon quantum dots (QDs) are considered among the most promising technologies for building scalable quantum computers. For this goal, ultra-low-power on-chip cryogenic CMOS (cryo-CMOS) electronics for control, read-out, and interfacing of the qubits is an important milestone. We report on-chip interfacing of tunable electron and hole QDs by a 64-channel cryo-CMOS multiplexer with less-than-detectable static power dissipation. We analyze charge noise and measure state-of-the-art addition energies and gate lever arm parameters in the QDs. We correlate low noise in QDs and sharp turn-on characteristics in cryogenic transistors, both fabricated with the same gate stack. Finally, we demonstrate that our hybrid quantum-CMOS technology provides a route to scalable interfacing of a large number of QD devices, enabling, for example, variability analysis and QD qubit geometry optimization, which are prerequisites for building large-scale silicon-based quantum computers.

Quantitative photocurrent scanning probe microscopy on PbS quantum dot monolayers.

Photoconductive atomic force microscopy can probe monolayers of PbS/perovskite quantum dots (QDs) with a contact area of 1-3 QDs in stable and reproducible acquisition conditions for I/V curves and photocurrent maps. From the measurements, quantitative values for the barrier height, built-in voltage, diffusion constant and ideality factor are deduced with high precision. The data analysis is based on modelling a superposition of the drift current of the photo-excited charges and a diffusion current across the interface barriers, providing physical insight into the underlying processes. Besides looking into PbS/perovskite on an indium tin oxide substrate, it is shown how the photocurrent is modified by changing either the QD ligand (to thiocyanate) or the substrate (to micro- and nanostructured gold). The dependence of the photocurrent on the light irradiance is found to follow a power law with an exponent of 0.64. Generally, quantitative measurements with high spatial resolution (on the single QD level) can provide significant insight into the processes in nanostructured hybrid optoelectronic components.

Fast and Artifact-Free Excitation Multiplexing Using Synchronized Image Scanning.

Multicolor fluorescence microscopy is an essential tool to visualize structures and dynamics in the life and materials sciences. However, the near-simultaneous acquisition of labels differing in excitation spectrum is difficult and renders such measurements prone to artifacts. We present a simple strategy to provide quasi-simultaneous fluorescence imaging with multiple excitation wavelengths by using an optical element to displace the sample image on the sensor at a rate that is much faster than the image acquisition rate and synchronizing this with the illumination. The emission elicited by the different wavelengths can then be encoded into the point-spread function of the imaging or visualized as multiple distinct images. In doing so, our approach can eliminate or mitigate artifacts caused by temporal aliasing in conventional sequential imaging. We demonstrate the use of our system to uncover hidden emissive states in single quantum dots and for the imaging of Ca2+ signaling in neurons.

Electronic States of Single Perovskite Quantum Dots in Weak and Strong Interaction Regimes: Implications in Electrically Pumped Quantum Emitters.

We investigate the effect of Coulomb interactions on the electronic states of a single perovskite quantum dot (PQD), CsPbBr3, through scanning tunneling microscopy/spectroscopy (STM/S). Under a weak interaction regime, where the time-averaged occupation of electrons in a PQD remains zero, the peaks observed in the differential tunneling conductance (dI/dV) spectrum correspond to the single-particle density of states (DOS) without any electron-electron correlation. However, with a shorter tunnel distance between the STM tip and PQD, additional electrons are trapped in the QD, leading to a strong interaction regime with well-defined electronic fine structures due to the lifting of spin degeneracy in the conduction bands. Interestingly, we observe that the strong Coulomb interaction can modify the spin-orbit coupling (SOC) strength in the PQDs. We have concluded that the energy levels under a strong electron-electron interaction regime are of utmost importance since they will be applicable to electrically pumped PQD-based single photon quantum emitters.

Direct observation of a few-photon phase shift induced by a single quantum emitter in a waveguide

Realizing a sensitive photon-number-dependent phase shift on a light beam is required both in classical and quantum photonics. It may lead to new applications for classical and quantum photonics machine learning or pave the way for realizing photon-photon gate operations. Nonlinear phase-shifts require efficient light-matter interaction, and recently quantum dots coupled to nanophotonic devices have enabled near-deterministic single-photon coupling. We experimentally realize an optical phase shift of 0.19π ± 0.03 radians ( ≈ 34 degrees) using a weak coherent state interacting with a single quantum dot in a planar nanophotonic waveguide. The phase shift is probed by interferometric measurements of the light scattered from the quantum dot in the waveguide. The process is nonlinear in power, the saturation at the single-photon level and compatible with scalable photonic integrated circuitry. The work may open new prospects for realizing high-efficiency optical switching or be applied for proof-of-concept quantum machine learning or quantum simulation demonstrations.

Quantum Dot/TiO2 Nanocomposite-Based Photoelectrochemical Sensor for Enhanced H2O2 Detection Applied for Cell Monitoring and Visualization.

This workexploits the possibility of using CdSe/ZnS quantum dot (QD)-electrodes to monitor the metabolism of living cells based on photoelectrochemical (PEC) measurements. To realize that, the PEC setup is improved with respect to an enhanced photocurrent signal, better stability, and an increased signal-to-noise ratio, but also for a better biocompatibility of the sensor surface on which cells have been grown. To achieve this, a QD-TiO2 heterojunction is introduced with the help of atomic layer deposition (ALD). The heterojunction reduces the charge carrier recombination inside the semiconductor nanoparticles and improves the drift behavior. The PEC performance is carefully analyzed by adjusting the TiO2 thickness and combining this strategy with multilayer immobilizations of QDs. The optimal thickness of this coating is ≈5nm; here, photocurrent generation can be enhanced significantly (e.g., for a single QD layer electrode by more than one order of magnitude at 0V vs Ag/AgCl). The resulting optimized electrode is used for hydrogen peroxide (H2O2) sensing with a good sensitivity down to µmolar concentrations, reusability, stability, response rate, and repeatability. Finally, the sensing system is applied to monitor the activity of cells directly grown on top of the electrode surface.

Reproduction of single-to-double hysteresis transition of nuclear spin polarization in a single InAlAs quantum dot

We have observed a transition from single to double hysteresis of nuclear spin polarization (NSP) with increasing magnetic field in a single InAlAs self-assembled quantum dot, which means the birth of a third stable branch that depends on the field strength. This NSP transition behavior could not be reproduced by standard model calculations using a fixed electron–nuclear spin correlation time τc under different external field conditions. By introducing the field dependence of τc, we were able to successfully reproduce the observed NSP transition. This finding on the phenomenological description of the magnetic field dependence will be a future highlight of τc.

Ligand Controls Excited Charge Carrier Dynamics in Metal-Rich CdSe Quantum Dots: Computational Insights.

Small metal-rich semiconducting quantum dots (QDs) are promising for solid-state lighting and single-photon emission due to their highly tunable yet narrow emission line widths. Nonetheless, the anionic ligands commonly employed to passivate these QDs exert a substantial influence on the optoelectronic characteristics, primarily owing to strong electron-phonon interactions. In this work, we combine time-domain density functional theory and nonadiabatic molecular dynamics to investigate the excited charge carrier dynamics of Cd28Se17X22 QDs (X = HCOO-, OH-, Cl-, and SH-) at ambient conditions. These chemically distinct but regularly used molecular groups influence the dynamic surface-ligand interfacial interactions in Cd-rich QDs, drastically modifying their vibrational characteristics. The strong electron-phonon coupling leads to substantial transient variations at the band edge states. The strength of these interactions closely depends on the physicochemical characteristics of passivating ligands. Consequently, the ligands largely control the nonradiative recombination rates and emission characteristics in these QDs. Our simulations indicate that Cd28Se17(OH)22 has the fastest nonradiative recombination rate due to the strongest electron-phonon interactions. Conversely, QDs passivated with thiolate or chloride exhibit considerably longer carrier lifetimes and suppressed nonradiative processes. The ligand-controlled electron-phonon interactions further give rise to the broadest and narrowest intrinsic optical line widths for OH and Cl-passivated single QDs, respectively. Obtained computational insights lay the groundwork for designing appropriate passivating ligands on metal-rich QDs, making them suitable for a wide range of applications, from blue LEDs to quantum emitters.

Universality and the thermoelectric transport properties of a double quantum dot system: Seeking for conditions that improve the thermoelectric efficiency

Employing universal relations for the Onsager coefficients in the linear regime at the symmetric point of the single impurity Anderson model, we calculate the conditions under which the quantum scattering phase shift should satisfy to produce the asymptotic Carnot’s limit for the thermoelectric efficiency. We show that a single quantum dot connected by metallic leads at the Kondo regime cannot achieve the best thermoelectric efficiency. We study a serial double quantum dot system, with the quantum dots immersed in ballistic conduction channels. Each QD exhibits a strong but finite local electronic correlation UU. We show that maintaining one dot in the electron-hole symmetric point and allowing charge fluctuations in the other QD makes it possible to drive the system to the maximum thermoelectric efficiency. We also show that the bound states in the continuum (BICs) and quasi-BICs associated with the quantum scattering interference process drive the DQD to the maximum thermoelectric efficiency. We identify two types of quasi-BICs that occur at low and high temperatures: The first is associated with single Fano resonances, and the last is with several Fano processes. We also discussed possible temperature values and conditions that could be linked with the experimental realization of the results.

Diameter-dependent whispering gallery mode lasing effects in quantum dot micropillar cavities

Whispering gallery mode (WGM) based microlasers have gained significant interest across various fields of nanophotonics, including biosensing, metrology, and on-chip excitation of single quantum dots in integrated quantum photonic structures. In this study, we report a comprehensive diameter-dependent study of whispering gallery mode lasing in quantum dot micropillar cavities. The lasing threshold, mode energy, quality factor, light-matter interaction in terms of the Purcell factor, and the free spectral range, are studied systematically for diameters ranging from 1 to 20 µm at cryogenic temperatures. To describe the experimental data, we use rate equation fitting and numerical simulations based on the finite element method, including realistic loss channels. Our results show a strong and systematic dependence of all lasing properties on the diameter of the micropillars. We also observe significant variations in the lasing properties of nominally identical micropillars, indicating a significant influence of the growth and fabrication imperfections on the output of the devices. The study provides important information on the optical properties of micropillar-based WGM lasing, which can aid in the advancement of optoelectronic applications using these nanophotonic structures.

Telecom Photon Emitters Based on Isolated Group-IV Quantum Dots Deterministically Coupled to High-Q Photonic Crystal Cavities

The realization of scalable telecom light emitters that can be monolithically implemented into large-scale Si integration technology has been a driving factor in the field of Si photonics for the last decades. Applications are envisioned in the short and medium-range data transfer and for realizing scalable, Si-based quantum information technology. For the latter, CMOS-compatible sources that can be controlled on the single photon level are needed. In solid-state materials, group-III-V quantum dots (QDs) are one of the leading platforms for realizing single photon emitters of excellent optical quality [1,2]. However, their emission outside the telecom band and the difficulty of combining them with the mature Si photonics components such as waveguides remain an ongoing problem.In the group-IV (SiGe) system, the bandgap of the bulk materials is indirect, and electron and hole states in QDs are spatially separated due to the type-II band alignment. These material properties lead to relatively long radiative lifetimes and small emission efficiencies. However, for Si/SiGe QDs grown on silicon on insulator substrates (SOI), these efficiencies can be strongly and deterministically Purcell-enhanced by aligning photonic crystal cavities with single QDs [3]. One necessary prerequisite is, therefore, to achieve perfect nucleation site control of the QDs on the substrates [4,5]. This nucleation control can be achieved by deterministic substrate patterning combined with Ge growth in the supersaturation regime of the two-dimensional wetting layer [6], utilizing Ge's extensive surface diffusion lengths at growth temperatures above 600°C [7]. In such a way, it is possible to grow isolated QDs with virtually arbitrary inter-QD distance [4,5].Here, one isolated QD was grown on a substrate area of the size of 100´100 µm2 [8]. We demonstrate the accurate QD positioning in PhC cavities [3,8], particularly in bichromatic cavities. Bichromatic cavities, a relatively novel design of photonic crystal cavity, offer ultra-high quality factor, and therefore Purcell enhancement, that is achievable with simple design rules [9]. Unlike in standard line defect cavities, in the present bichromatic layout, the line defect consists of a periodic sequence of holes, leaving only narrow Si regions.For this reason, an extremely high accuracy for QD positioning is required, which can be provided by interlacing site control of QD growth and PhC cavity formation. In micro photoluminescence spectra, the modes of single cavities are clearly observed. From the dependence of the mode intensities on the temperature and the excitation intensity, modes fed by the single QD in the cavity can be identified. We observe ultra-high quality factors of up to 100,000 for the modes coupled to QDs [8]. For resonators loaded with a QD, such high Q-factor values are record-high for the silicon-on-insulator integrated optics platform. Results on the excited state lifetime will be discussed.[1] D. Huber et al., Phys. Rev. Lett. 121, 33902 (2018)[2] N. Somaschi et al., Nature Photonics 10, 340 (2016)[3] M. Schatzl et al., ACS Photonics 4, 665 (2017)[4] M. Grydlik et al., Nanotechnology 24, 105601 (2013)[5] M. Brehm, et al., Nanotechnology 28, 392001 (2017)[6] M. Brehm, et al., Physical Review B 80 (20), 205321 (2009)[7] M. Grydlik et al., Physical Review B 88 (11), 115311 (2013)[8] T. Poempool et al., Optics Express 31 (10), 15564-15578 (2023)[9] A. Simbula et al., APL Photonics 2, 056102 (2017).

Robust consistent single quantum dot strong coupling in plasmonic nanocavities

Strong coupling between a single quantum emitter and an optical cavity (at rate Ω) accesses fundamental quantum optics and provides an essential building block for photonic quantum technologies. However, the minimum mode volume of conventional dielectric cavities restricts their operation to cryogenic temperature for strong coupling. Here we harness surface self-assembly to make deterministic strong coupling at room temperature using CdSe/CdS quantum dots (QDs) in nanoparticle-on-mirror (NPoM) plasmonic nanocavities. We achieve a fabrication yield of ~70% for single QD strong coupling by optimizing their size and nano-assembly. A clear and reliable Rabi splitting is observed both in the scattering of each nanocavity and their photoluminescence, which are however not equal. Integrating these quantum elements with electrical pumping allows demonstration of strong coupling in their electroluminescence. This advance provides a straightforward way to achieve practical quantum devices at room temperature, and opens up exploration of their nonlinear, electrical, and quantum correlation properties.

(Invited) Photoluminescence Properties of Single InAsP Quantum Dots Embedded in InP Nanowires

Non-classical light emitters that can generate single photons with a negligible multiphoton probability are one of the key components for quantum information technologies. Deterministically grown III-V semiconductor nanowires containing quantum dots are gaining interest as a viable platform for quantum key distribution applications. In this talk, we will report on our recent development of the fabrication of InAsP single quantum dots embedded within InP photonic waveguide nanowires. In particular, we outline the importance of the photonic waveguide design for optimum photon generation and coupling to external optics [1]. The measured count rate dependence on normalized wire diameter, D/λ (figure 1) of the nanowire sources is consistent with calculations of the spontaneous emission rate into the fundamental HE11 nanowire waveguide mode (ΓHE11). Manipulating dot growth conditions and engineering the band structure around the dot (dot-in-a-rod configuration) are applied [2] to enhance the photoluminescence emission rate at 1310 nm and 1550 nm. Single photon emission with very low multiple photon probability is demonstrated at O- and C-band [3,4]. Temperature dependent, second-order correlation measurements on the 1310 nm source show that these nanowire sources can generate single photons up to temperatures of 220 K [3].[1] S. Haffouz, et al., Nano Letters, 18, 3047 (2018).[2] S. Haffouz, et al., Applied Physics Letters, 117, 113101 (2020).[3] P. Laferriére, et al., Nano Letters, 23, 962 (2023).[4] A.N. Wakileh, et al., arXiv:2309.13381 (2023). Figure 1

Plasmon Mediated Single Photon Emission from a Nanocrystal Ensemble.

Quantum photonic devices require robust sources of single photons to perform basic computational and communication protocols. Thus, developing scalable, integrable, and efficient quantum light sources has become crucial for the realization of quantum photonic devices. Single quantum dots are promising sources of quantum light due to their tunable emission wavelength. Here, we show the emergence of quantum-emitter-like antibunched emission behavior when multiple quantum dots are located in the vicinity of plasmonic particles. To evaluate the robustness of this phenomenon, we consider both monometallic and bimetallic particles. We find that the photoluminescence intensity of the plasmon coupled quantum dots fits well to a single sublinear power law exponent that is distinct from the behavior of CQD aggregates. Significantly, we find that plasmon coupling results in reduced flickering, thus enabling the realization of a more stable and reliable single photon source. Possible roles of emergent excitonic interactions in the coupled system are discussed.