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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 217 records · Page 12
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Indium–Poly(carboxylic acid) Ligand Interactions Modify InP Quantum Dot Nucleation and Growth

Size control through precursor reactivity in InP quantum dot (QD) synthesis has been difficult due to the presence of kinetically persistent InP clusters when using conventional indium carboxylate and tris(trimethylsilyl)phosphine chemistry. However, the advent of indium halide/aminophosphine-based synthesis creates new opportunities to harness precursor design to impact nucleation and growth. Driven to further explore indium coordination as a synthetic handle in InP QD synthesis, we examined the effect of a strongly chelating anion on the nucleation and growth of InP QDs. Increasing the equivalents of metal-chelating aminopoly(carboxylic acid) EDTA ([CH 2 N(CH 2 CO 2 H) 2 ] 2 ) (0–0.75 equiv per indium) is found to decrease the final diameter of InP QDs from 4.5 to 2.3 nm by lowering the initial InP growth rate. This size trend is rationalized by invoking a continuous nucleation model. Control experiments carried out with substoichiometric equivalents of indium do not exhibit a drastic size decrease, pointing to complex effects of EDTA on the indium precursor reactivity. By 1 H NMR spectroscopy, EDTA is identified to form an octahedral complex with indium that is less reactive. Furthermore, this competitive decrease in reactivity and in the effective concentration of indium precursor is proposed to suppress the initial InP growth rates and consequently decrease the final size of the nanocrystals.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Uncovering the Role of Hole Traps in Promoting Hole Transfer from Multiexcitonic Quantum Dots to Molecular Acceptors

The understanding of electronic dynamics in multiexcitonic quantum dots (QDs) is important for designing efficient systems useful in high power scenarios, such as solar concentrators and multielectron charge transfer. The multiple charge carriers within a QD can undergo undesired Auger recombination events, which rapidly annihilate carriers on picosecond time scales and generate heat from absorbed photons instead of useful work. Compared to the transfer of multiple electrons, the transfer of multiple holes has proven to be more difficult due to slower hole transfer rates. To probe the competition between Auger recombination and hole transfer in CdSe, CdS, and CdSe/CdS QDs of varying sizes, we synthesized a phenothiazine derivative with optimized functionalities for binding to QDs as a hole accepting ligand and for spectroscopic observation of hole transfer. Transient absorption spectroscopy was used to monitor the photoinduced absorption features from both trapped holes and oxidized ligands under excitation fluences where the averaged initial number of excitons in a QD ranged from ~1 to 19. We observed fluence-dependent hole transfer kinetics that last around 100 ps longer than the predicted Auger recombination lifetimes, and the transfer of up to 3 holes per QD. Theoretical modeling of the kinetics suggests that binding of hole acceptors introduces trapping states significantly different from those in native QDs passivated with oleate ligands. Holes in these modified trap states have prolonged lifetimes, which promotes the hole transfer efficiency. These results highlight the beneficial role of hole-trapping states in devising hole transfer pathways in QD-based systems under multiexcitonic conditions.

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

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↗
DOE OSTI2024

Multilayered luminescent solar concentrators based on engineered quantum dots

Luminescent solar concentrators (LSCs) based on engineered quantum dots (QDs) are disclosed that include at least one lower band-gap energy LSC layer and at least one higher band-gap energy LSC layer. The higher band-gap energy LSC layer has a higher internal quantum efficiency (IQE) than the lower band-gap energy LSC layer. The lower band-gap energy LSC layer may broadly absorb the remainder of the solar spectrum that is not absorbed by previous layers. An external optical efficiency (EQE) of at least 6%, and in some cases, more than 10%, may be achieved by such LSCs.

Source record↗
DOE OSTI2020

Multimode description of self-mode locking in a single-section quantum-dot laser

This paper describes a theory for mode locking and frequency comb generation by four-wave mixing in a semiconductor quantum-dot active medium. The derivation uses a multimode semiclassical laser theory that accounts for fast carrier collisions within an inhomogeneous distribution of quantum dots. Numerical simulations are presented to illustrate the role of active medium nonlinearities in mode competition, gain saturation, carrier-induced refractive index and creation of combination tones that lead to locking of beat frequencies among lasing modes in the presence of cavity material dispersion.

Chow, Weng W.↗
DOE OSTI2025

Crystalline-symmetry-protected Majorana modes in coupled quantum dots

We propose a minimalist architecture for achieving various crystalline-symmetry-protected Majorana modes in an array of coupled quantum dots. Our framework is motivated by the recent experimental demonstrations of two-site and three-site artificial Kitaev chains in a similar setup. We find that introducing a π-phase domain wall in the Kitaev chain leads to a pair of mirror-protected Majorana zero modes located at or near the junction. Joining two π junctions into a closed loop, we can simulate two distinct classes of two-dimensional higher-order topological superconducting phases, both carrying symmetry-protected Majorana modes around the sample corners. As an extension of the π junction, we further consider a general vertex structure where n Kitaev chains meet, i.e., a Kitaev n vertex. We prove that such an n vertex, if respecting a dihedral symmetry group D n , necessarily carries n vertex-bound Majorana modes protected by the D n symmetry. Resilience of the junction and vertex Majorana bound states against disorder and correlation effects is also discussed. Our architecture paves the way for designing, constructing, and exploring a wide variety of artificial topological crystalline phases in quantum-dot experiments.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRS2017

Device and Method of Scintillating Quantum Dots for Radiation Imaging

A radiation imaging device includes a radiation source and a micro structured detector comprising a material defining a surface that faces the radiation source. The material includes a plurality of discreet cavities having openings in the surface. The detector also includes a plurality of quantum dots disclosed in the cavities. The quantum dots are configured to interact with radiation from the radiation source, and to emit visible photons that indicate the presence of radiation. A digital camera and optics may be used to capture images formed by the detector in response to exposure to radiation.

Burke, Eric R.↗
DOE OSTI2021

Semiconductor quantum dots: Technological progress and future challenges

In quantum-confined semiconductor nanostructures, electrons exhibit distinctive behavior compared with that in bulk solids. This enables the design of materials with tunable chemical, physical, electrical, and optical properties. Zero-dimensional semiconductor quantum dots (QDs) offer strong light absorption and bright narrowband emission across the visible and infrared wavelengths and have been engineered to exhibit optical gain and lasing. These properties are of interest for imaging, solar energy harvesting, displays, and communications. Here, we offer an overview of advances in the synthesis and understanding of QD nanomaterials, with a focus on colloidal QDs, and discuss their prospects in technologies such as displays and lighting, lasers, sensing, electronics, solar energy conversion, photocatalysis, and quantum information.

García de Arquer, F. Pelayo↗
NASA NTRS2012

Complementary Barrier Infrared Detector (CBIRD) with Double Tunnel Junction Contact and Quantum Dot Barrier Infrared Detector (QD-BIRD)

The InAs/GaSb type-II superlattice based complementary barrier infrared detector (CBIRD) has already demonstrated very good performance in long-wavelength infrared (LWIR) detection. In this work, we describe results on a modified CBIRD device that incorporates a double tunnel junction contact designed for robust device and focal plane array processing. The new device also exhibited reduced turn-on voltage. We also report results on the quantum dot barrier infrared detector (QD-BIRD). By incorporating self-assembled InSb quantum dots into the InAsSb absorber of the standard nBn detector structure, the QD-BIRD extend the detector cutoff wavelength from approximately 4.2 micrometers to 6 micrometers, allowing the coverage of the mid-wavelength infrared (MWIR) transmission window. The device has been observed to show infrared response at 225 K.

antimonide↗
DOE OSTI2022

Two-band optical gain and ultrabright electroluminescence from colloidal quantum dots at 1000 A cm−2

Abstract Colloidal quantum dots (QDs) are attractive materials for the realization of solution-processable laser diodes. Primary challenges towards this objective are fast optical-gain relaxation due to nonradiative Auger recombination and poor stability of colloidal QD solids under high current densities required to obtain optical gain. Here we resolve these challenges and achieve broad-band optical gain spanning the band-edge (1S) and the higher-energy (1P) transitions. This demonstration is enabled by continuously graded QDs with strongly suppressed Auger recombination and a current-focusing device design, combined with short-pulse pumping. Using this approach, we achieve ultra-high current densities (~1000 A cm −2 ) and brightness (~10 million cd m −2 ), and demonstrate an unusual two-band electroluminescence regime for which the 1P band is more intense than the 1S feature. This implies the realization of extremely large QD occupancies of up to ~8 excitons per-dot, which corresponds to complete filling of the 1S and 1P electron shells.

47 OTHER INSTRUMENTATION↗
DOE OSTI2025

Nonequilibrium steady-state thermoelectrics of Kondo-correlated quantum dots

The transport across a Kondo-correlated quantum dot coupled to two leads with independent temperatures and chemical potentials is studied using a controlled nonperturbative, and in this sense numerically exact, treatment based on a hybrid numerical renormalization group combined with time-dependent density matrix renormalization group (NRG-tDMRG). In the Kondo regime, for sufficiently large fixed voltage bias V ≳ T K , with T K the Kondo temperature, we find a peak in the conductance vs the temperature gradient Δ⁢T = T R - T L across left and right lead. Focusing then on zero voltage bias but finite ΔT far beyond linear response, we reveal the dependence of the characteristic zero-bias conductance on the individual lead temperatures. Here, we find that the finite-Δ⁢T data behaves quantitatively similar to linear response with an effective equilibrium temperature derived from the different lead temperatures. The regime of sign changes in the Seebeck coefficient, signaling the presence of Kondo correlations, and its dependence on the individual lead temperatures provide a complete picture of the Kondo regime in the presence of finite-temperature gradients. The results from the zero-bias conductance and Seebeck coefficient studies unveil an approximate “Kondo circle” in the T L /T R plane as the regime within which the Kondo correlations dominate. We also study the heat current and the corresponding heat conductance vs finite Δ⁢T. We provide a polynomial fit for our numerical results for the thermocurrent as a function of the individual lead temperatures, which may be used to fit experimental data in the Kondo regime.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRS2001

Quantum Dots Based Rad-Hard Computing and Sensors

Quantum Dots (QDs) are solid-state structures made of semiconductors or metals that confine a small number of electrons into a small space. The confinement of electrons is achieved by the placement of some insulating material(s) around a central, well-conducting region. Thus, they can be viewed as artificial atoms. They therefore represent the ultimate limit of the semiconductor device scaling. Additional information is contained in the original extended abstract.

Fijany, A.↗
DOE OSTI2020

Cadmium sulfide quantum dots

Provided herein are compositions comprising cadmium sulfide quantum dot photocatalysts and methods and systems utilizing as much (e.g., for the reduction of a nitrobenzene to an aniline).

77 NANOSCIENCE AND NANOTECHNOLOGY↗
NASA NTRS2003

Lasing characteristics of InAs quantum dot laers on InP substrate

Single-stack InAs self-assembled quantum dots (QD) lasers based on InP substrate have been grown by metalorganic vapor phase epitaxy. The narrow ridge waveguide lasers lased up to 260 K in continuous wave operation, and near room temperature in pulsed mode, with wavelengths between 1.59 to 1.74 mu m.

quantum dot semiconductor laser↗
DOE OSTI2022

A room-temperature polarization-sensitive CMOS terahertz camera based on quantum-dot-enhanced terahertz-to-visible photon upconversion

Detection of terahertz (THz) radiation has many potential applications, but presently available detectors are limited in many aspects of their performance, including sensitivity, speed, bandwidth and operating temperature. Most do not allow the characterization of THz polarization states. Recent observation of THz-driven luminescence in quantum dots offers a possible detection mechanism via field-driven interdot charge transfer. Here, we demonstrate a room-temperature complementary metal–oxide–semiconductor THz camera and polarimeter based on quantum-dot-enhanced THz-to-visible upconversion mechanism with optimized luminophore geometries and fabrication designs. Besides broadband and fast responses, the nanoslit-based sensor can detect THz pulses with peak fields as low as 10 kV cm–1. A related coaxial nanoaperture-type device shows a to-date-unexplored capability to simultaneously record the THz polarization state and field strength with similar sensitivity.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2024

Ligand-Induced Size-Dependent Circular Dichroism in Quantum Dots

Recent experiments have probed the chiral properties of semiconductor nanocrystal (NC) quantum dots (QDs), but understanding the circular dichroism line shape, excitonic features, and chirality induction mechanism remains a challenge. We propose an atomistic pseudopotential method to model chiral ligand passivated QDs, computing circular dichroism (CD) spectra for CdSe QDs (2.6-3.8 nm). We find strong agreement between calculated and measured line shapes, predicting consistent bisignate line shapes with decreasing CD magnitude as size increases. Further, our analysis reveals the origin of bisignate line shapes, arising from nondegenerate excitons with opposing angular momenta. We also explore the impact of chiral ligand orientation on QD surfaces, observing changes in the optical activity magnitude and sign. This orientation sensitivity offers the means to distinguish ordered from disordered ligand configurations, facilitating the study of order-disorder transitions at ligand-QD interfaces.

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

Synthesis of PbS/CdS/Cu 2-x S core/shell/shell quantum dots for rapid NIR emission.

Nanoscale semiconductors, known as quantum dots (QDs), possess unique size-tunable optical and electrical properties. With continued research into quantum information storage and quantum communication, the need for near-infrared single photon emitters and absorbers has gained prominence. Lead sulfide QDs have only recently been explored as a reliable near-infrared single photon emitters with the addition of a protective cadmium sulfide shell. Despite the increased air and room temperature stability of these QDs, long photon emission times have limited widespread application. This work examines the enhanced photon emission due to the Purcell effect provided by the layering of copper sulfide. In particle, this work synthesized lead sulfide cores in the 10 nm range, successfully layered cadmium sulfide through cation exchange, and attempted the cation exchange of copper sulfide, as identified with near-infrared absorbance spectra, transmission electron microscopy, and photoluminescence spectra.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Exciton-Phonon Coupling and Carrier Relaxation in PbS Quantum Dots: The Case of Carboxylate Ligands

Some ligand-nanocrystal combinations exhibit rapid cooling of highly excited electronic states while other nanocrystal/shell combinations do not appear to have this effect. There remains a need to identify the distinguishing properties of ligand-nanocrystal interactions that avoid such rapid relaxation processes to guide the design of colloidal quantum dots (QDs) that take advantage of multiple exciton generation or hot-carrier extraction processes. Here, we use mid-infrared transient absorption spectroscopy to investigate the influence that carboxylate ligands with distinct excited state surface chemistries has on exciton-phonon coupling and hot exciton relaxation in PbS quantum dot (QD) films. Our findings reveal that despite significant differences in the excited state surface chemistry of oleate (OA) and iodide/mercaptopropionic acid (I-/MPA) ligands, PbS QD films passivated with both ligand types exhibit identical electronic relaxation rates and exciton-phonon coupling strengths within experimental precision. The data suggest that the inorganic lattice is the principal source of exciton-phonon coupling that influences hot exciton relaxation, rather than the vibronic modes of carboxylate ligands. The size-dependent nature of the exciton-phonon coupling strength is consistent with the localization of charge on the QD surfaces, which enhances the mixing of electronic and nuclear coordinates particularly when the electronic states are more quantum confined in smaller nanocrystals.

14 SOLAR ENERGY↗