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At least 163 records · Page 9

Prospects and challenges of colloidal quantum dot laser diodes

Colloidal quantum dots (QDs) combine the superior light-emission characteristics of quantum-confined semiconductors with the chemical flexibility of molecular systems. We find that these properties could, in principle, enable solution-processable laser diodes with an ultrawide range of accessible colours. However, the realization of such devices has been hampered by fast optical gain decay due to non-radiative Auger recombination and poor stability of QD solids at the high current densities required for the lasing regime. Recently, these problems have been resolved, which resulted in the development of electrically pumped optical gain devices operating at ultrahigh current densities of around 1,000 A cm -2 . The next step is the realization of a QD laser diode (QLD). Here we assess the status of the QD lasing field, examine the remaining challenges on the path to a QLD and discuss practical strategies for attaining electrically pumped QD lasing.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Observation of biexciton emission from single semiconductor nanoplatelets

Quasi-two-dimensional semiconductor nanoplatelets (NPLs) are intriguing systems for studying the influence of Auger recombination processes on the multiexciton emission efficiencies in the weak in-plane confinement regime. We investigate CdSe/CdS core/shell NPLs using cryogenic temperature single particle spectroscopy and observe bright biexciton emission at high excitation powers. The average binding energy of the biexcitons is determined to be 16.5 meV. The observed switching between the biexciton and trion states indicates charging-decharging dynamics of the NPLs mediated by the Auger ionization process. These findings are highly relevant for harvesting efficient biexciton emission for energy, lighting, and quantum applications.

36 MATERIALS SCIENCE↗

Control of light-matter interactions in hybrid structured environments with novel nanomaterials of different dimensionalities

The project calls for exploration of individual nanomaterials and the ability to fabricate functional structures without degrading the properties of components. The rich photophysics of novel semiconductors like transition metal dichalcogenides (TMDs), lead halide perovskites (LHPs) and nanocrystal quantum dots (NQDs) can be gainfully exploited in integrated photonic structures alongside conventional semiconducting and dielectric materials. Realization of the prospects of such hybrid structures crucially depends on the ability to fabricate these “designer” assemblies while preserving and enhancing the optoelectronic properties of individual components. We study emission properties of these materials at both bulk and single particles levels to elucidate their intrinsic photophysical properties in order to minimize energy losses and facilitate their judicious integration via control of energy/charge flows and photon-exciton interconversions.

36 MATERIALS SCIENCE↗

Confinement of excited states in two-dimensional, in-plane, quantum heterostructures

Two-dimensional (2D) semiconductors are promising candidates for optoelectronic application and quantum information processes due to their inherent out-of-plane 2D confinement. In addition, they offer the possibility of achieving low-dimensional in-plane exciton confinement, similar to zero-dimensional quantum dots, with intriguing optical and electronic properties via strain or composition engineering. However, realizing such laterally confined 2D monolayers and systematically controlling size-dependent optical properties remain significant challenges. Here, we report the observation of lateral confinement of excitons in epitaxially grown in-plane MoSe 2 quantum dots (~15-60 nm wide) inside a continuous matrix of WSe 2 monolayer film via a sequential epitaxial growth process. Various optical spectroscopy techniques reveal the size-dependent exciton confinement in the MoSe 2 monolayer quantum dots with exciton blue shift (12-40 meV) at a low temperature as compared to continuous monolayer MoSe 2 . Finally, single-photon emission (g 2 (0) ~ 0.4) was also observed from the smallest dots at 1.6 K. Our study opens the door to compositionally engineered, tunable, in-plane quantum light sources in 2D semiconductors.

42 ENGINEERING↗

Dangling Bonds as Possible Contributors to Charge Noise in Silicon and Silicon–Germanium Quantum Dot Qubits

Spin qubits based on Si and Si 1–x Ge x quantum dot architectures exhibit among the best coherence times of competing quantum computing technologies, yet they still suffer from charge noise that limit their qubit gate fidelities. Identifying the origins of these charge fluctuations is therefore a critical step toward improving Si quantum-dot-based qubits. Here, we use hybrid functional calculations to investigate possible atomistic sources of charge noise, focusing on charge trapping at Si and Ge dangling bonds (DBs). We evaluate the role of global and local environment in the defect levels associated with DBs in Si, Ge, and Si 1–x Ge x alloys, and consider their trapping and excitation energies within the framework of configuration coordinate diagrams. We additionally consider the influence of strain and oxidation in charge-trapping energetics by analyzing Si and GeSi DBs in SiO 2 and strained Si layers in typical Si 1–x Ge x quantum dot heterostructures. Our results identify that Ge dangling bonds are more problematic charge-trapping centers both in typical Si 1–x Ge x alloys and associated oxidation layers, and they may be exacerbated by compositional inhomogeneities. In conclusion, these results suggest the importance of alloy homogeneity and possible passivation schemes for DBs in Si-based quantum dot qubits and are of general relevance to mitigating possible trap levels in other Si, Ge, and Si 1–x Ge x -based metal-oxide-semiconductor stacks and related devices.

36 MATERIALS SCIENCE↗

Electrically driven light emission from single quantum dots using pulsed MOS capacitors

Robust, nanoscale light-emitting devices are attractive for emerging photonic and quantum engineering applications. However, conventional approaches suffer from fabrication challenges or lack the potential to address individual nanostructures, such as quantum dots. In this paper, we present a device that can produce electrically driven light emission from a single quantum dot using a single carbon nanotube as the charge injection contact. Here, the device has a metal-oxide-semiconductor capacitor structure and operates based on an unconventional mechanism of electroluminescence, which relies on the use of bipolar voltage pulses. The proposed device can be fabricated in a simple manner using conventional lithographic processes, offering a scalable approach toward the development of optoelectronic devices at the single dot level.

42 ENGINEERING↗

Tracking Thermal Transport in Colloidal Quantum Dot Films Using in Situ Time-Resolved X-ray Diffraction

Colloidal quantum dots (QDs) and their thin films are increasingly used in electronic and photonic devices replacing traditional bulk semiconductors. However, thermal properties of QDs remain underexplored relative to device development efforts. This study shows the use of time-resolved X-ray diffraction as a contact-free method to probe the thermal response of QDs in environments representative of the active layer in QD optoelectronic devices, providing in situ insights for future thermal management strategies. Through the extraction of Debye–Waller factors on a subnanosecond time scale, we directly capture the heating and cooling of core/shell CdSe/CdS QDs following pulsed optical excitation. In a QD thin film that actively provides optical gain, the thermal conductivity is found to be as low as 0.13 W m –1 K –1 , because of the poor heat flow between close-packed QD solids. For QDs dispersed in liquids, interfacial thermal conductance dominates thermal relaxation, with a conductance of 15 MW m –2 K –1 .

36 MATERIALS SCIENCE↗

Spontaneous Exciton Collapse in a Strongly Flattened Ellipsoidal InSb Quantum Dot

Abstract Electronic and excitonic states in an InSb strongly flattened ellipsoidal quantum dot (QD) with complicated dispersion law are theoretically investigated within the framework of the geometric adiabatic approximation in the strong, intermediate, and weak quantum confinement regimes. For the lower levels of the spectrum, the square root dependence of energy on QD sizes is revealed in the case of Kane’s dispersion law. The obtained results are compared to the case of a parabolic (standard) dispersion law of charge carriers. The possibility of the accidental exciton instability is revealed for the intermediate quantum confinement regime. For the weak quantum confinement regime, the motion of the exciton's center-of-gravity is quantized, which leads to the appearance of additional Coulomb-like sub-levels. It is revealed that in the case of the Kane dispersion law, the Coulomb levels shift into the depth of the forbidden band gap, moving away from the quantum confined level, whereas in the case of the parabolic dispersion law, the opposite picture is observed. The corresponding selection rules of quantum transitions for the interband absorption of light are obtained. New selection rules of quantum transitions between levels conditioned by 2D exciton center of mass vertical motion quantization in a QD are revealed. The absorption threshold behavior characteristics depending on the QDs geometrical sizes are also revealed.

97 MATHEMATICS AND COMPUTING↗

Metal-Tipped and Electrochemically Wired Semiconductor Nanocrystals: Modular Constructs for Directed Charge Transfer

In our 2017 proposal to the Solar Photochemistry division of DOE/BES/Office of Science we targeted the creation, characterization and integratation of new II-IV semiconductor heterostructured nanomaterials into ultra-thin film (tethered) nanocrystalline arrays on transparent metal oxide (TCO) supports. Materials were to include CdSe quantum dots (QDs), asymmetric CdSe@CdS tetrapods (TPs) and CdSe@CdS nanorods (NRs), into unique photoelectrochemical platforms. The ultimate goal was to tether these new nanomaterials to either electron- or hole-selective oxide interlayers that would afford vectoral photo-induced charge transfer and ultimately formation of molecular products such as H 2 . This was an ambitious set of goals but integrated well with our previous work in this general area.

14 SOLAR ENERGY↗

Zero-bias conductance peaks at zero applied magnetic field due to stray fields from integrated micromagnets in hybrid nanowire quantum dots

Many recipes for realizing topological superconductivity rely on broken time-reversal symmetry, which is often attained by applying a substantial external magnetic field. Alternatively, using magnetic materials can offer advantages through low-field operation and design flexibility on the nanoscale. Mechanisms for lifting spin degeneracy include exchange coupling, spin-dependent scattering, spin injection – all requiring direct contact between the bulk or induced superconductor and a magnetic material. Here, we implement locally broken time-reversal symmetry through dipolar coupling from nearby micromagnets to superconductor-semiconductor hybrid nanowire devices. Josephson supercurrent is hysteretic due to micromagnets switching. At or around zero external magnetic field, we observe an extended presence of Andreev bound states near zero voltage bias. We also show a zero-bias peak plateau of a non-quantized value. Our findings largely reproduce earlier results where similar effects were presented in the context of topological superconductivity in a homogeneous wire, and attributed to more exotic time-reversal breaking mechanisms [Nat. Phys. 17, 43 (2020)]. In contrast, our stray field profiles are not designed to create Majorana modes, and our data are compatible with a straightforward interpretation in terms of trivial states in quantum dots. At the same time, the use of micromagnets in hybrid superconductor-semiconductor devices shows promise for future experiments on topological superconductivity.

Jiang, Luyao [Univ. of Pittsburgh, PA (United Stat↗

Nanorod length-dependent photodriven H2 production in 1D CdS–Pt heterostructures

Colloidal quantum confined semiconductor-metal heterostructures are promising candidates for solar energy conversion because their light absorbing semiconductor and catalytic components can be independently tuned and optimized. Although the light-to-hydrogen efficiencies of such systems have shown interesting dependences on the morphologies of the semiconductor and metal domains, the mechanisms of such dependences are poorly understood. Here, we use Pt tipped 0D CdS quantum dots (with ∼4.6 nm diameter) and 1D CdS nanorods (of ∼13.8, 27.8, 66.6, and 88.9 nm average rod lengths) as a model system to study the distance-dependence of charge separation and charge recombination times and their impacts on photo-driven H2 production. The H2 generation quantum efficiency increases from 0.2% ± 0.0% in quantum dots to 28.9% ± 0.4% at a rod length of 28 nm and shows negligible changes at longer rod lengths. The half-life time of electron transfer from CdS to Pt increases monotonically with rod length, from 0.7 ± 0.1 in quantum dots to 170.2 ± 29.5 ps in the longest rods, corresponding to a slight decrease in electron transfer quantum efficiency from 92% to 81%. The amplitude-weighted average lifetime of charge recombination of the electron in Pt with the hole in CdS increases from 4.7 ± 0.4 µs in quantum dots to 149 ± 34 µs in 28 nm nanorods, and the lifetime does not increase further in longer rods, resembling the trend in the observed H2 generation quantum efficiency. Our result suggests that the competition of the charge recombination process with the hole removal by the sacrificial electron donor plays a dominant role in the observed nanorod length dependent overall light driven H2 generation quantum efficiency.

Chemistry↗

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, in this work, 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.

biexciton↗

Device response principles and the impact on energy resolution of epitaxial quantum dot scintillators with monolithic photodetector integration

Abstract Epitaxial quantum dot (QD) scintillator crystals with picosecond-scale timing and high light yield have been created for medical imaging, high energy physics and national security applications. Monolithic photodetector (PD) integration enables the sensing of photons generated within the waveguiding crystal and allows a wide range of scintillator-photodetector coupling geometries. Until recently, these doubly novel devices have suffered from complex, high variance responses to monoenergetic sources which significantly reduces their precision and accuracy. The principles governing the overall device response have now been discerned and embodied by an expression derived within a geometrical optics framework which considers optical properties, surface roughness and photodetector coupling geometry. Response variation due to these factors was sufficiently reduced to obtain material-related energy resolution values of 2.4% with alpha particles. These findings place energy resolution alongside luminescence timescale, photon yield, and radiation hardness as outstanding properties of these engineered materials.

36 MATERIALS SCIENCE↗

Valley splitting correlations across a silicon quantum well containing germanium

Quantum dots in SiGe/Si/SiGe heterostructures host coherent electron spin qubits, which are promising for future quantum computers. The silicon quantum well hosts near-degenerate electron valley states, creating a low-lying excited state that is known to reduce spin qubit readout and control fidelity. The valley energy splitting is dominated by the microscopic disorder in the SiGe alloy and at the Si/SiGe interfaces, and while Si devices are compatible with large-scale semiconductor manufacturing, achieving a uniformly large valley splitting energy across a many-qubit device spanning mesoscopic distances is an outstanding challenge. In this work we study valley splitting variations in a 1D quantum dot array, formed in a Si 0.972 Ge 0.028 quantum well, manufactured by Intel. We observe correlations in valley splitting, at both sub-100 nm (single gate) and > 1 μm (device) lengthscales, that are consistent with alloy disorder-dominated theory and simulation. Our results develop the mesoscopic understanding of Si/SiGe heterostructures necessary for scalable device design.

Marcks, Jonathan C. [Argonne National Laboratory (↗

PbE (E = S, Se) Colloidal Quantum Dot-Layered 2D Material Hybrid Photodetectors

Hybrid lead chalcogenide (PbE) (E = S, Se) quantum dot (QD)-layered 2D systems are an emerging class of photodetectors with unique potential to expand the range of current technologies and easily integrate into current complementary metal-oxide-semiconductor (CMOS)-compatible architectures. Herein, we review recent advancements in hybrid PbE QD-layered 2D photodetectors and place them in the context of key findings from studies of charge transport in layered 2D materials and QD films that provide lessons to be applied to the hybrid system. Photodetectors utilizing a range of layered 2D materials including graphene and transition metal dichalcogenides sensitized with PbE QDs in various device architectures are presented. Figures of merit such as responsivity (R) and detectivity (D*) are reviewed for a multitude of devices in order to compare detector performance. Finally, a look to the future considers possible avenues for future device development, including potential new materials and device treatment/fabrication options.

36 MATERIALS SCIENCE↗

Atomically dispersed Pb ionic sites in PbCdSe quantum dot gels enhance room-temperature NO2 sensing

Abstract Atmospheric NO 2 is of great concern due to its adverse effects on human health and the environment, motivating research on NO 2 detection and remediation. Existing low-cost room-temperature NO 2 sensors often suffer from low sensitivity at the ppb level or long recovery times, reflecting the trade-off between sensor response and recovery time. Here, we report an atomically dispersed metal ion strategy to address it. We discover that bimetallic PbCdSe quantum dot (QD) gels containing atomically dispersed Pb ionic sites achieve the optimal combination of strong sensor response and fast recovery, leading to a high-performance room-temperature p-type semiconductor NO 2 sensor as characterized by a combination of ultra–low limit of detection, high sensitivity and stability, fast response and recovery. With the help of theoretical calculations, we reveal the high performance of the PbCdSe QD gel arises from the unique tuning effects of Pb ionic sites on NO 2 binding at their neighboring Cd sites.

36 MATERIALS SCIENCE↗

Method for fabricating embedded nanostructures with arbitrary shape

A layered heterostructure, comprising alternating layers of different semiconductors, wherein one of the atom species of one of the semiconductors has a faster diffusion rate along an oxidizing interface than an atom species of the other semiconductor at an oxidizing temperature, can be used to fabricate embedded nanostructures with arbitrary shape. The result of the oxidation will be an embedded nanostructure comprising the semiconductor having slower diffusing atom species surrounded by the semiconductor having the higher diffusing atom species. The method enables the fabrication of low- and multi-dimensional quantum-scale embedded nanostructures, such as quantum dots (QDs), toroids, and ellipsoids.

Wang, George T.↗