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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Low-threshold laser medium utilizing semiconductor nanoshell quantum dots

Colloidal semiconductor nanocrystals (NCs) represent a promising class of nanomaterials for lasing applications. Currently, one of the key challenges facing the development of high-performance NC optical gain media lies in enhancing the lifetime of biexciton populations. This usually requires the employment of charge-delocalizing particle architectures, such as core/shell NCs, nanorods, and nanoplatelets. Here, we report on a two-dimensional nanoshell quantum dot (QD) morphology that enables a strong delocalization of photoinduced charges, leading to enhanced biexciton lifetimes and low lasing thresholds. A unique combination of a large exciton volume and a smoothed potential gradient across interfaces of the reported CdS bulk /CdSe/CdS shell (core/shell/shell) nanoshell QDs results in strong suppression of Auger processes, which was manifested in this work though the observation of stable amplified stimulated emission (ASE) at low pump fluences. An extensive charge delocalization in nanoshell QDs was confirmed by transient absorption measurements, showing that the presence of a bulk-size core in CdS bulk /CdSe/CdS shell QDs reduces exciton–exciton interactions. Altogether, present findings demonstrate unique advantages of the nanoshell QD architecture as a promising optical gain medium in solid-state lighting and lasing applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Fano Resonance in CO 2 Reduction Catalyst Functionalized Quantum Dots

Molecular catalyst functionalized semiconductor quantum dots (QDs) are a promising modular platform for developing novel hybrid photocatalysts. The interaction between adsorbed catalyst vibrations and the QD electron intraband absorption can influence the photophysical properties of both the QD and the catalysts and potentially their photocatalysis. In CdSe QDs functionalized by the CO 2 reduction catalyst, Re(CO) 3 (4,4’-bipyridine-COOH)Cl, we observe that the transient Fano resonance signal resulting from coupling of the catalyst CO stretching mode and the QD conduction band electron mid-IR intraband absorption appears on an ultrafast time scale and decays with the electron population, irrespective of the occurrence of photoreduced catalysts. The Fano asymmetry factor increases with an increase in the adsorbed catalyst number and a decrease in QD sizes. The latter can be attributed to an enhanced charge transfer interaction between the more strongly quantum-confined QD conduction band and catalyst LUMO levels. These results provide a more in-depth understanding of interactions in excited QD-catalyst hybrid photocatalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Atomistically resolved hot exciton relaxation dynamics in CdSe quantum dots: Experiment and theory

Semiconductor quantum dots (QDs) are well known to give rise to a quantum confined structure of excitons. Because of this quantum confinement, new physics of hot exciton relaxation dynamics arises. Decades of work using transient absorption (TA) spectroscopy have yielded initial simple observations, such as estimates of the cooling rate from single pump photon energy experiments. More detailed TA experiments employed variable pump photon energies to measure excitonic state-resolved transition rates. These TA measurements, usually the simplest form, have been employed to characterize QDs and their relaxation dynamics to this day. Yet, these TA measurements are fundamentally lacking in their ability to measure energy-resolved hot exciton cooling, which requires observation of the full cooling history through the real excitonic manifold. Here, we employ coherent multi-dimensional spectroscopy (CMDS) to perform an atomistically directed study of hot exciton cooling in CdSe QDs, revealing energy resolved relaxation dynamics. CMDS experiments are compared with simulations and prior TA measurements and simpler theories. Our findings reveal a hot exciton relaxation dynamics landscape. This relaxation dynamics landscape is a linear or sub-linear function of excess energy for different structures of QDs, with a strong size dependence. Our model simulations parameterized by the empirical pseudopotential model reproduces the experimental functional form and the dependence upon QD diameter and shell.

Atomistic simulations↗
DOE OSTI2023

Combined Coherent Manipulation and Single-Shot Measurement of an Electron Spin in a Quantum Dot (Final Technical Report)

Semiconductor quantum dots (QDs) are promising candidates to act as single-photon sources and/or quantum bits in future optical quantum information applications. Their excellent optical properties such as high brightness, single-photon purity, and narrow linewidth have potential utility in many areas. One challenge is to control the energy levels of the QD without using a magnetic field. The AC Stark effect offers the opportunity to do this. We have demonstrated record-large AC Stark shifts of the energy states of a single charged QD. We showed that the shifts can be applied in a spin-selective manner by controlling the polarization of the laser producing the AC Stark effect. In order to characterize the effect, we developed a novel spectral filtering scheme to discriminate the high-power AC Stark laser from the QD fluorescence. We also developed a compact, low-cost, homemade polarimeter to help control the polarization of the AC Stark laser, which enabled the spin selectivity of the AC Stark effect. With the practical capabilities thus developed, we learned that the spin-selective AC Stark effect causes electron spin pumping, which in turn causes nuclear spin pumping via the hyperfine interaction. The nuclear spin pumping causes a mean field Zeeman interaction between the nuclear spin ensemble and the electron trapped in the QD, resulting in the so-called Overhauser shift. The magnitude of the Overhauser shift and the measured linewidth of the QD’s optical transitions enabled characterization of the mean nuclear spin polarization and fluctuations. The potentially rapid (ns-scale) control of the QD energy levels and nuclear spin polarization will enable measurements of electron and nuclear spin polarization in the absence of any real magnetic field, which is a completely unique capability. The ability to rapidly apply a spin-selective AC Stark effect in the presence of a weak real magnetic field will allow control of the polarization selection rules of the transitions, enabling all single-qubit operations on the electron spin, i.e., initialization, coherent manipulation, and quantum non-demolition measurement.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2025

Pressure-Modulated Energy Transfer Dynamics in Mn 2+ -Doped CdS/ZnS Core/Shell Quantum Dots

Transition metal doping in semiconductor quantum dots (QDs) significantly impacts their optical properties, thus expanding the range of their potential optoelectronic applications. This study investigates the pressure-dependent energy transfer dynamics in Mn 2+ -doped CdS/ZnS core/shell QDs, focusing on how external hydrostatic pressure modulates these dynamics and optical properties. By synthesizing Mn 2+ -doped QDs with varying Mn 2+ doping concentrations, we explore the effects of the pressure on photoluminescence (PL) spectra and energy transfer efficiency. Our study reveals that increasing pressure induces a blueshift in the QD host bandgap PL and a redshift in the Mn 2+ dopant PL. The pressure-induced shifts highlight a unique modulation mechanism where the energy transfer efficiency decreases with pressure due to reduced wave function overlap between host excitons and Mn 2+ dopants. Detailed analysis of the PL quantum yields and energy transfer rate constants provides insights into these dynamics, suggesting that the pressure can effectively and reversibly regulate the energy transfer efficiencies and rates. In conclusion, these results have implications for developing pressure-sensitive configurable devices and exploring pressure-induced phenomena in doped nanomaterials.

36 MATERIALS SCIENCE↗
NASA NTRS2003

Fluorescent Quantum Dots for Biological Labeling

Fluorescent semiconductor quantum dots that can serve as "on/off" labels for bacteria and other living cells are undergoing development. The "on/off" characterization of these quantum dots refers to the fact that, when properly designed and manufactured, they do not fluoresce until and unless they come into contact with viable cells of biological species that one seeks to detect. In comparison with prior fluorescence-based means of detecting biological species, fluorescent quantum dots show promise for greater speed, less complexity, greater sensitivity, and greater selectivity for species of interest. There are numerous potential applications in medicine, environmental monitoring, and detection of bioterrorism.

McDonald, Gene↗
DOE OSTI2020

Rugged nanoparticle tracers for mass tracking in explosive events

Tracing the flow of solid matter during an explosion requires a rugged tag that can be measured by a unique identifiable signature. Silica-covered semiconductor quantum dots (QDs) provide a unique and tunable photoluminescent signature that emits from within a sacrificial outer layer. Five types of silica-covered zinc sulfide QDs were synthesized and covalently bound to commercial luminescent powders. The combination of five dots and five powders enables a matrix of 25 unique tags. The tracers are shown to be tolerant of environments associated with chemical explosives and provides a unique tag to evaluate debris fields.

45 MILITARY TECHNOLOGY, WEAPONRY, AND NATIONAL DEF↗
DOE OSTI2025

Role of Superlattice Phonons in Charge Localization Across Quantum Dot Arrays

Understanding charge transport in semiconductor quantum dot (QD) assemblies is important for developing the next generation of solar cells and light-harvesting devices based on QD technology. One of the key factors that governs the transport in such systems is related to the hybridization between the QDs. Recent experiments have successfully synthesized QD molecules, arrays, and assemblies by directly fusing the QDs, with enhanced hybridization leading to high carrier mobilities and coherent band-like electronic transport. Here, in this work, we theoretically investigate the electron transfer dynamics across a finite CdSe-CdS core-shell QD array, considering up to seven interconnected QDs in one dimension. We find that, even in the absence of structural and size disorder, electron transfer can become localized by the emergent low-frequency superlattice vibrational modes when the connecting neck between QDs is narrow. On the other hand, we also identify a regime where the same vibrational modes facilitate coherent electron transport when the connecting necks are wide. Overall, we elucidate the crucial effects of electronic and superlattice symmetries and their couplings when designing high-mobility devices based on QD superlattices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Analog Quantum Simulation of the Dynamics of Open Quantum Systems with Quantum Dots and Microelectronic Circuits

We introduce a general setup for the analog quantum simulation of the dynamics of open quantum systems based on semiconductor quantum dots electrically connected to a chain of quantum RLC electronic circuits. The dots are chosen to be in the regime of spin-charge hybridization to enhance their sensitivity to the RLC circuits while mitigating the detrimental effects of unwanted noise. In this context, we establish an experimentally realizable map between the hybrid system and a qubit coupled to thermal harmonic environments of arbitrary complexity that enables the analog quantum simulation of open quantum systems. We assess the utility of the simulator by numerically exact emulations that indicate that the experimental setup can faithfully mimic the intended target even in the presence of its natural inherent noise. We further provide a detailed analysis of the physical requirements on the quantum dots and the RLC circuits needed to experimentally realize this proposal that indicates that the simulator can be created with existing technology. The approach can exactly capture the effects of highly structured non-Markovian quantum environments typical of photosynthesis and chemical dynamics, and offer clear potential advantages over conventional and even quantum computation. The proposal opens a general path for effective quantum dynamics simulations based on semiconductor quantum dots.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Cross-correlation spectra in interacting quantum dot systems

Two-color spin-noise spectroscopy of interacting electron spins in singly charged semiconductor quantum dots provides information on the interquantum dot interactions. We investigate the spin cross-correlation function in a quantum dot ensemble employing a modified semiclassical approach. Spin-correlation functions are calculated using a Hamilton quaternion approach that maintains local quantum mechanical properties of the spins. This method takes into account the effects of the nuclear-electric quadrupolar interactions, the randomness of the coupling constants, and the variation of the electron g factor on the spin-noise power spectra. We demonstrate that the quantum dot ensemble can be mapped on an effective two-quantum dot problem and discuss how the characteristic length scale of the interdot interaction modifies the low-frequency cross-correlation spectrum. Here, we argue that details on the interaction strength distribution can be extracted from the cross-correlation spectrum when applying a longitudinal or a transversal external magnetic field.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Performance of Scintillation Detectors Based on Quantum Dots in a Semiconductor Matrix (Final Technical Report)

InAs Quantum Dots (QDs) embedded into GaAs semiconductor waveguide have unique scintillation properties, valuable for nuclear security, medical imaging, and high energy physics. In this work, we developed thick (~25um) epitaxial heterostructres with high luminescence efficiency composed of self-assembled nano-engineered InAs QDs grown by molecular beam epitaxy. In this type of detector, the GaAs matrix acts as a stopping material for charged particles or photons generating electrons captured by the QDs acting as luminescence centers. The QD medium is designed to provide fast capture of electrons into QDs (few ps), high QD luminescence efficiency at room temperature (>50%), and strong red-shift of photoluminescence (PL) from the GaAs absorption edge (>250nm). Typical devices consist of a 10-25um thick GaAs layer with embedded sheets of modulation p-type doped InAs QDs and an InGaAs photodetector tuned to the QD emission wavelength. The thick GaAs layer acts also as a waveguide when layer-transferred onto a low-index substrate. Waveguiding and self-absorption (~1cm -1 ) were studied using photoluminescence with scanning laser excitation and modeled with ray optics approximation and geometrical coupling of high-index waveguide to a collection fiber. Scintillating signals from α-particles were analyzed with both an external photodiode (PD) and an integrated PD which provided an improved optical coupling. In the former case, the external InGaAs PD was air-coupled to the scintillator and had the light collection efficiency of about 1% corresponding to limited light extraction through a planar interface with air due to total internal reflection. The mean charge collected by the integrated PD was in the range of (3÷5)×10 4 photoelectrons per 1 MeV of deposited energy, or ~13-20% of the theoretically achievable light yield. Timing of the integrated device was measured by wire-bonding it to the input of an 8 GHz IC. The scintillation response shows an extremely fast 0.3-0.6 ns decay constant and about 40-70 ps time resolution, limited by the system noise. The combined light yield and decay time makes the InAs/GaAs QD heterostructures the fastest high yield scintillation material reported making it valuable for high energy physics and medical imaging applications.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2021

Ambient Tip-Enhanced Photoluminescence with 5 nm Spatial Resolution

We achieve record spatial resolution in ambient tip-enhanced photoluminescence (TEPL) from CdSe/ZnS semiconductor quantum dots (QDs). Our approach only takes advantage of surface roughness at the apex of a sputtered plasmonic gold probe. When irradiated with visible light (633 and 532 nm lasers), nano-corrugated regions of the apex of an Au tip support 5-nm spatial resolution in TEPL imaging of QD aggregates on silicon. The reproducibility of our observations is illustrated using different plasmonic probes and samples. The origin of the observed near-field contrast, underlying the demonstrated high spatial resolution in TEPL, is discussed in the context of field enhancement at the metal tip-fluorophore interface.

Chemical Dynamics Initiative↗
DOE OSTI2020

Distinguishing Electron and Hole Dynamics in Functionalized CdSe/CdS Core/Shell Quantum Dots Using Complementary Ultrafast Spectroscopies and Kinetic Modeling

The evolution of excitation energy and photogenerated charges in semiconductor quantum dots (QDs) functionalized with molecular acceptors can be probed on ultrafast time scales using techniques such as transient absorption (TA) spectroscopy. However, historical interpretations that the 1S(e)-1S 3/2 (h) transition in Cd-chalcogenide QDs is fully attributable to electrons may be misleading, and multiexponential models used to fit TA kinetics do not correspond directly to specific photophysical processes. Here, we present visible-wavelength and mid-IR TA and time-resolved photoluminescence measurements to inform a comprehensive kinetic model of the photoexcited CdSe/CdS core/shell QDs functionalized with passivating oleic acid (OA), hole-accepting ferrocene, or electron-accepting naphthalene bisimide (NBI). We show that ~30% of the 1S signal and 72% of the IR signal can originate from holes in well-passivated core/shell QDs. We also demonstrate evidence of electron trapping in OA-capped core/shell QDs, with additional electron transfer and hole trapping in the QDs functionalized with NBI. Electron (hole) trapping and detrapping occur in 450 ± 100 ps (430 ± 70 ps) and 340 ± 100 ps (1.1 ± 0.4 ns) respectively, while the time constant for electron transfer to NBI is ~1.8 ns. The comprehensive picture of photophysical processes provided by the complementary ultrafast techniques and kinetic modeling can accelerate both the fundamental science and application development of nanostructured and molecular systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Quantum simulation of an exotic quantum critical point in a two-site charge Kondo circuit

Tuning a material to the cusp between two distinct ground states can produce physical properties that are unlike those in either of the neighbouring phases. Advances in the fabrication and control of quantum systems have raised the tantalizing prospect of artificial quantum simulators that can capture such behaviour. A tunable array of coupled qubits should have an appropriately rich phase diagram, but realizing such a system with either tunnel-coupled semiconductor quantum dots or metal nanostructures has proven difficult. The challenge for scaling up to clusters or lattices is to ensure that each element behaves essentially identically and that the coupling between elements is uniform, while also maintaining tunability of the interactions. Here we study a nanoelectronic circuit comprising two coupled hybrid metal–semiconductor islands, combining the strengths of both materials to form a potentially scalable platform. The semiconductor component allows for controllable inter-site couplings at quantum point contacts, while the metal component’s effective continuum of states means that different sites can be made equivalent by tuning local potentials. The couplings afforded by this architecture can realize an unusual quantum critical point resulting from frustrated Kondo interactions. In this study, the observed critical behaviour matches theoretical predictions, verifying the success of our experimental quantum simulation.

36 MATERIALS SCIENCE↗