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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 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

Optical Two-Dimensional Spectroscopy of Semiconductor Quantum Wells and Quantum Dots (Final Report)

The goal of this program was to implement optical 2-dimensional coherent spectroscopy and apply it to electronic excitations, including excitons, in semiconductors. Specif ically of interest were epitaxially grown quantum wells that exhibit disorder due to well width fluctuations and quantum dots. In both cases, 2-D spectroscopy provided information regarding coupling among excitonic localization sites. In the first year of the project, a significant fraction of our progress was on quantum wells, rather than quantum dots, which have been more our focus in recent years. The two main results were 1) providing an understanding of the polarization dependence of the homogeneous linewidth in quantum wells based on using an anharmonic boson model, and 2) using multidimensional spectroscopy to observe spectral diffusion due to exciton migration amongst within localized states due to disorder.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2022

Technoeconomic Model Suggests Scaling-Up Perovskite Quantum Dots for Optoelectronics Warrants Improved Synthesis Yield, Solvent Recycling, and Automation

A comprehensive technoeconomic cost-analysis of perovskite quantum dot optoelectronics is reported. Using economies-of-scale considerations based on price data from prominent materials suppliers, higher QD synthesis yield, solvent recycling, and synthesis automation are shown to be critical for market-entry of this technology. Combinedly, this three-pronged approach drives quantum dot film fabrication costs down from >$50/m 2 to ~$2-3/m 2 .

14 SOLAR ENERGY↗
DOE OSTI2025

Geometry-driven modeling of electron localization in InAs/GaAs double quantum dots

The coupled electronic states in two-dimensional (2D) and three-dimensional (3D) double quantum dot (DQD) systems are investigated using a phenomenological model applied to InAs/GaAs heterostructures. The single-band k • p effective potential approach previously proposed by our group is employed to numerically calculate the energy spectrum and spatial localization of a single electron, serving as an indicator of the coupling strength within the binary system. For identical quantum dots (QDs) in a DQD, the electronic states exhibit ideal coherence. We systematically vary the DQD geometry and the strength of the confinement potential (via an applied electric field) to examine the effects of symmetry breaking and the sensitivity of electron localization in both identical and nearly identical DQDs. Our results show that coherence in DQDs is highly sensitive to these subtle variations. This sensitivity can be harnessed to detect changes in the surrounding environment, such as fluctuations in chemical or electrical properties that affect the DQD system.

electron localization↗
DOE OSTI2023

Stable Cadmium-Free Quantum Dot Optical Down-Converters for Solid State Lighting

Quantum dots (QDs) have been used in commercial solid-state lighting (SSL) applications to improve the energy efficiency of light generation at warm color temperatures. By increasing the amount of QDs used in each product, further energy savings are possible; however, traditional QDs contain cadmium, which has regulatory limits on its concentration in consumer products. As described within this final technical report, we have established that heavy-metal free QDs made from indium phosphide (InP) exhibit highly efficient emission at the temperatures and fluxes relevant to SSL. However, the maintenance of this emission is compromised during long term operation due to QD oxidation. We have identified multiple methods to slow the oxidation rate, which has improved the operational stability of these materials more than 200 times longer than at the project start. Beyond these improvements, heavy-metal free QDs require a further hundred-fold increase in stability to enable use in mid-power SSL and a ten-fold increase in stability to enable use in diffuse SSL applications. The outcomes of this project demonstrate feasibility for the use of heavy-metal free QDs in commercial SSL applications with potential use in diffuse SSL applications in the near term (1-2 years) pending market need.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2020

Surface Ligand Management Aided by a Secondary Amine Enables Increased Synthesis Yield of CsPbI 3 Perovskite Quantum Dots and High Photovoltaic Performance

Lead-halide perovskite quantum dots (PQDs) or more broadly, nanocrystals possess advantageous features for solution-processed photovoltaic devices. The nanocrystal surface ligands play a crucial role in the transport of photogenerated carriers and ultimately affect the overall performance of PQD solar cells. Here, significantly improved CsPbI 3 PQD synthetic yield and solar-cell performance through surface ligand management are demonstrated. The treatment of a secondary amine, di- n -propylamine (DPA), provides a mild and efficient approach to control the surface ligand density of PQDs, which has an apparently different working mechanism compared to previously reported surface treatments. Using an optimal DPA concentration, the treatment can simultaneously remove both long-chain insulating surface ligands of oleic acid and oleylamine, even for unpurified PQDs with high ligand density. As a result, the electrical coupling between PQDs is enhanced, leading to improved charge transport, reduced carrier recombination, and a high power conversion efficiency approaching 15% for CsPbI 3 -PQD-based solar cells. In addition, the production yield of CsPbI 3 PQDs can be increased by a factor of 8. These results highlight the importance of developing new ligand-management strategies, specifically for emerging PQDs to achieve scalable and high-performance perovskite-based optoelectronic devices.

36 MATERIALS SCIENCE↗
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 OSTI2026

Photoinduced Charge Transfer and Vibronic Coherence in CdSe Quantum Dots with Methyl Viologen Acceptors

We show herein that photoinduced charge transfer from CdSe quantum dots (QDs) to surface-bound methyl viologen (MV 2+ ) acceptors is mediated by a vibronically coherent, nonadiabatic mechanism. Broadband multidimensional electronic spectra and an analysis of coherences show that a mixed QD–MV charge-transfer (CT) state is populated on the <50 fs time scale after optical preparation of the X3 (1P 3/2 –1P e ) state, well prior to the appearance of the one-electron photoreduced ground state (MV +• ). A partial redistribution of charge from the core of the QD to the acceptor is revealed by excited-state coherences of an out-of-plane vibrational mode local to MV 2+ and of a low-frequency mode mixing a MV 2+ mode with the longitudinal optical (LO) phonon of the QD core. The ultrafast damping of these coherences indicates that excited-state wavepackets travel from the optically prepared, Franck–Condon structure through a conical intersection to reach the CT state. These results suggest that vibronically coherent processes generating CT intermediates can be exploited to improve the efficiency of QD-based solar cells and photocatalysts.

Cadmium selenide↗
DOE OSTI2023

Quantifying the Variation in the Number of Donors in Quantum Dots Created Using Atomic Precision Advanced Manufacturing

Atomic-precision advanced manufacturing enables unique silicon quantum electronics built on quantum dots fabricated from small numbers of phosphorus dopants. The number of dopant atoms comprising a dot plays a central role in determining the behavior of charge and spin confined to the dots and thus overall device performance. Here in this work, we use both theoretical and experimental techniques to explore the combined impact of lithographic variation and stochastic kinetics on the number of P incorporations in quantum dots made using these techniques and how this variation changes as a function of the size of the dot. Using a kinetic model of PH3 dissociation augmented with novel reaction barriers, we demonstrate that for a 2 × 3 silicon dimer window the probability that no donor incorporates goes to zero, allowing for certainty in the placement of at least one donor. However, this still comes with some uncertainty in the precise number of incorporated donors (either one or two), and this variability may still impact certain applications. We also examine the impact of the size of the initial lithographic window, finding that the incorporation fraction saturates to δ-layer-like coverage as the circumference-to-area ratio decreases. We predict that this incorporation fraction depends strongly on the dosage of the precursor and that the standard deviation of the number of incorporations scales as ~√n, as would be expected for a sequence of largely independent incorporation events. Finally, we characterize an array of 36 experimentally prepared multidonor 3 × 3 nm lithographic windows with scanning tunneling microscopy, measuring the fidelity of the lithography to the desired array and the final location of PH x fragments within these lithographic windows. We use our kinetic model to examine the expected variability due to the observed lithographic error, predicting a negligible impact on incorporation statistics. We find good agreement between our model and the inferred incorporation locations in these windows from scanning tunneling microscope measurements.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Colloidal Quantum Dot Photovoltaics: Current Progress and Path to Gigawatt Scale Enabled by Smart Manufacturing

Colloidal quantum dots (QDs) have lately been pursued with intense vigor for optoelectronic applications such as photovoltaics (PV), flexible electronics, displays, mid-infrared photodetectors, lasers, and single-photon emitters. These nanometer-sized semiconducting crystals can be suitably mass-produced and size-tuned via cost-effective solution-based synthetic routes to operate in the quantum size confinement regime, endowing them with a wide array of exotic optical and electronic properties. While the first potential market entry could be in displays and in niche applications such as “internet-of-things”, ultimately, the technology has the potential to influence large-scale terrestrial power generation, because it is amenable to high-throughput synthesis from Earth-abundant materials and large-area solution-based coating techniques and can be air-stable. In this Review, we chronicle the recent advances that have propelled QD PV toward commercialization and highlight potential areas for further progress. We present an account of the material compositions being explored as QDs and their various benefits, major chemical passivation and doping strategies that have been developed to allay QD surface traps, and advanced device designs deployed to maximize charge extraction. We also discuss pathways to >20% efficient QD PV and describe recent advances in high-precision and autonomous synthesis of such materials. With recent demonstrations of scalable synthesis of high-quality QDs, smart manufacturing of QDs and QD solids, and fabrication of stable solar cells under ambient conditions, we suggest that the technology is on the road to achieving maturity and technological relevance and that gigawatt per year distributed panel production sites may be within reach.

14 SOLAR ENERGY↗
DOE OSTI2024

Photoluminescence Switching in Quantum Dots Connected with Carboxylic Acid and Thiocarboxylic Acid End-Group Diarylethene Molecules

We contrast the switching of photoluminescence (PL) of PbS quantum dots (QDs) cross-linked with photochromic diarylethene molecules with different end groups, 4,4′-(1-cyclopentene-1,2-diyl)bis[5-methyl-2-thiophenecarboxylic acid] ( 1C ) and 4,4′-(1-cyclopentene-1,2-diyl)bis[5-methyl-2-thiophenethiocarboxylic acid] ( 2T ). Our results show that the QDs cross-linked with the carboxylic acid end group molecules ( 1C ) exhibit a greater amount of switching in photoluminescence intensity compared to QDs cross-linked with the thiocarboxylic acid end group ( 2T ). We also demonstrate that regardless of the molecule used, greater switching amounts are observed for smaller quantum dots. Varying these parameters allows for the fabrication of photoswitches with tunable PL change. We relate these observations to the differences in the HOMO energy levels between the QDs and the photochromic molecules. Our findings demonstrate how the size of the QDs and the energy levels of the linker ligands influences the charge tunneling rate and thus the PL switching performance in tunneling-based photoswitches.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Degradation mechanisms of 1.3 μm C-doped quantum dot lasers grown on native substrate

Here, the aim of this paper is to analyse the degradation modes of 1.3 μm InAs quantum dot laser diodes (QD LDs) grown by using carbon as a p-type dopant, as an alternative to beryllium. The devices were stressed at high current densities, to favor the onset of excited-state (ES) emission, and to study the related degradation phenomena. The study of QD LDs is of fundamental importance for the photonic integrated circuits (PICs). The investigation is based on two types of stress tests: 1) a current step stress and 2) a constant current stress. With these experiments we demonstrate that a) the current is a determining factor for the onset of the ES during the operation of such devices. b) the onset of ES is responsible for a rapid quenching of the ground state (GS) emission. c) stress induces a significant increase in the threshold current of the devices, that is ascribed to the lowering of the injection efficiency, which in turn can be explained by the easier escape of carriers from quantum dots (QDs) from ES energy levels. d) the contribution of defects on the optical and electrical degradation is also discussed.

42 ENGINEERING↗
DOE OSTI2021

Extending the Near-Infrared Emission Range of Indium Phosphide Quantum Dots for Multiplexed In Vivo Imaging

This report of the reddest emitting indium phosphide quantum dots (InP QDs) to date demonstrates tunable, near-infrared (NIR) photoluminescence (PL) as well as PL multiplexing in the first optical tissue window while avoiding toxic constituents. This synthesis overcomes the InP “growth bottleneck” and extends the emission peak of InP QDs deeper into the first optical tissue window using an inverted QD heterostructure, specifically ZnSe/InP/ZnS core/shell/shell nanoparticles. The QDs exhibit InP shell thickness-dependent tunable emission with peaks ranging from 515–845 nm. The high absorptivity of InP yields effective photoexcitation of the QDs with UV, visible, and NIR wavelengths. These nanoparticles extend the range of tunable direct-bandgap emission from InP-based nanostructures, effectively overcoming a synthetic barrier that has prevented InPbased QDs from reaching their full potential as NIR imaging agents. Further, multiplexed lymph node imaging in a mouse model demonstrates the potential of the NIR-emitting InP particles for in vivo imaging.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2022

Pit rim decomposition into multiple quantum dots on surfaces of epitaxial thin films grown on pit-patterned substrates

Here, we report results of dynamical simulations according to an experimentally validated surface morphological evolution model on the formation of regular arrays of quantum dot molecules (QDMs) consisting of 1D arrays of smaller interacting quantum dots (QDs). These QD arrays form along the sides of each pit rim on the surface of a coherently strained thin film epitaxially deposited on a semiconductor substrate, the surface of which consists of a periodic pattern of inverted prismatic pits with rectangular pit openings. We find that this complex QDM pattern results from the decomposition of the pit rim from a “quantum fortress” with four elongated QDs into four 1D arrays of multiple smaller QDs arranged along each side of the pit rim. Systematic parametric analysis indicates that varying the pit opening dimensions and the pit wall inclination directly impacts the number of QDs in the resulting QDM pattern, while varying the pit depth only affects the dimensions of the QDs in the nanostructure pattern. Therefore, the number, arrangement, and sizes of QDs in the resulting pattern of QDMs on the film surface can be engineered precisely by proper tuning of the pit design parameters. Our simulation results are supported by predictions of morphological stability analysis, which explains the pit rim decomposition into multiple QDs as the outcome of a tip-splitting instability and provides a fundamental characterization of the post-instability nanostructure pattern. Our theoretical findings can play a vital role in designing optimal semiconductor surface patterns toward enabling future nanofabrication technologies.

36 MATERIALS SCIENCE↗
DOE OSTI2024

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.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Imaging Quantum Interference in Stadium-Shaped Monolayer and Bilayer Graphene Quantum Dots

Experimental realizations of graphene-based stadium-shaped quantum dots (QDs) have been few and have been incompatible with scanned probe microscopy. Yet, the direct visualization of electronic states within these QDs is crucial for determining the existence of quantum chaos in these systems. Here we report the fabrication and characterization of electrostatically defined stadium-shaped QDs in heterostructure devices composed of monolayer graphene (MLG) and bilayer graphene (BLG). To realize a stadium-shaped QD, we utilized the tip of a scanning tunneling microscope to charge defects in a supporting hexagonal boron nitride flake. The stadium states visualized are consistent with tight-binding-based simulations but lack clear quantum chaos signatures. The absence of quantum chaos features in MLG-based stadium QDs is attributed to the leaky nature of the confinement potential due to Klein tunneling. In contrast, for BLG-based stadium QDs (which have stronger confinement) quantum chaos is precluded by the smooth confinement potential which reduces interference and mixing between states.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Physics and applications of quantum dot lasers for silicon photonics

Abstract Photonic integrated circuits (PICs) have enabled numerous high performance, energy efficient, and compact technologies for optical communications, sensing, and metrology. One of the biggest challenges in scaling PICs comes from the parasitic reflections that feed light back into the laser source. These reflections increase noise and may cause laser destabilization. To avoid parasitic reflections, expensive and bulky optical isolators have been placed between the laser and the rest of the PIC leading to large increases in device footprint for on-chip integration schemes and significant increases in packaging complexity and cost for lasers co-packaged with passive PICs. This review article reports new findings on epitaxial quantum dot lasers on silicon and studies both theoretically and experimentally the connection between the material properties and the ultra-low reflection sensitivity that is achieved. Our results show that such quantum dot lasers on silicon exhibit much lower linewidth enhancement factors than any quantum well lasers. Together with the large damping factor, we show that the quantum dot gain medium is fundamentally dependent on dot uniformity, but through careful optimization, even epitaxial lasers on silicon can operate without an optical isolator, which is of paramount importance for the future high-speed silicon photonic systems.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Elucidating the Location of Cd 2+ in Post-synthetically Treated InP Quantum Dots Using Dynamic Nuclear Polarization 31 P and 113 Cd Solid-State NMR Spectroscopy

Indium phosphide quantum dots (InP QD) are a promising alternative to traditional QD materials that contain toxic heavy elements such as lead and cadmium. However, InP QD obtained from colloidal synthesis are often plagued by poor photoluminescence quantum yields (PL-QYs). In order to improve the PL-QY of InP QD, a number of post-synthetic treatments have been devised. Recently, it has been shown that InP post-synthetically treated with Lewis acid metal divalent cations (M-InP) exhibit enhanced PL-QY; however, the molecular structure and mechanism behind the improved PL-QY are not fully understood. Here, to determine the surface structure of M-InP QD, dynamic nuclear polarization surface-enhanced nuclear magnetic resonance spectroscopy (DNP SENS) experiments were employed on a series of InP magic size clusters treated with Cd ions, InP QD, cadmium phosphide (Cd 3 P 2 ) QD, and Cd-treated InP QD (Cd–InP QD). With the use of DNP SENS, we were able to obtain the 1D 31 P and 113 Cd NMR spectra, 113 Cd{ 31 P} rotational-echo double-resonance (REDOR) NMR spectra, and 31 P{ 113 Cd} dipolar heteronuclear multiple quantum correlation (D-HMQC) sequence. Changes in the phosphide 31 P chemical shifts after Cd treatment provide indirect evidence that some Cd alloys into the sub-surface regions of the particle. DNP-enhanced 113 Cd solid-state NMR spectra suggest that most Cd ions are coordinated by oxygen atoms from either carboxylate ligands or surface phosphate groups. 113 Cd{ 31 P} REDOR and 31 P{ 113 Cd} D-HMQC experiments confirm that a subset of Cd ions are located on the surface of Cd–InP QD and coordinated with phosphate groups.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗