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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 55 records · Page 3
All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

Direct Nanoscale Characterization of Deep Levels in AgCuInGaSe 2 Using Electron Energy–Loss Spectroscopy in the Scanning Transmission Electron Microscope

A new experimental framework for the characterization of defects in semiconductors is demonstrated. Through the direct, energy-resolved correlation of three analytical techniques spanning six orders of magnitude in spatial resolution, a critical mid-bandgap electronic trap level (E V + 0.56 eV) within Ag 0.2 Cu 0.8 In 1–x Ga x Se 2 is traced to its nanoscale physical location and chemical source. This is achieved through a stepwise, site-specific correlated characterization workflow consisting of device-scale (≈1 mm 2 ) deep level transient spectroscopy (DLTS) to survey the traps present, scanning probe–based DLTS (scanning-DLTS) for mesoscale-resolved (hundreds of nanometers) mapping of the target trap state’s spatial distribution, and scanning transmission electron microscope based electron energy-loss spectroscopy (STEM-EELS) and X-ray energy-dispersive spectroscopy for nanoscale energy-, structure, and chemical-resolved investigation of the defect source. Furthermore, this first demonstration of the direct observation of sub-bandgap defect levels via STEM-EELS, combined with the DLTS methods, provides strong evidence that the longsuspected Cu In/Ga substitutional defects are indeed the most likely source of the E V + 0.56 eV trap state and serves as a key example of this approach for the fundamental identification of defects within semiconductors, in general.

14 SOLAR ENERGY↗
DOE OSTI2023

Detection of hot electrons originating from an upper valley at ∼1.7eV above the Γ valley in wurtzite GaN using electron emission spectroscopy

Using electron emission spectroscopy, measurement and analysis were conducted on the energy distribution of vacuum emitted electrons from electrically driven InGaN/GaN green (peak wavelengths 𝜆 ≈ 515nm) light-emitting diodes (LEDs) with and without a prewell superlattice (SL). Here, we report on the detection of a high-energy upper valley at ∼ 1.7eV above the Γ valley from samples with no prewell SL. We propose that these upper valley electrons originate predominantly from trap-assisted Auger recombination (TAAR) in green LEDs, as the intensity of these peaks is found to have quadratic dependence on the carrier density 𝑛 [see Espenlaub et al., J. Appl. Phys. 126, 184502 (2019)]. The high-energy upper valley peak was not observed in the sample with a prewell SL which is attributed to gettering by the prewell SL of still unidentified impurities that act as TAAR centers.

carrier generation & recombination↗
DOE OSTI2016

Electron holes in inhomogeneous magnetic field: Electron heating and electron hole evolution

Electron holes are electrostatic non-linear structures widely observed in the space plasma. In the present paper, we analyze the process of energy exchange between electrons trapped within electron hole, untrapped electrons, and an electron hole propagating in a weakly inhomogeneous magnetic field. We show that as the electron hole propagates into the region with stronger magnetic field, trapped electrons are heated due to the conservation of the first adiabatic invariant. At the same time, the electron hole amplitude may increase or decrease in dependence on properties of distribution functions of trapped and untrapped resonant electrons. The energy gain of trapped electrons is due to the energy losses of untrapped electrons and/or decrease of the electron hole energy. We stress that taking into account the energy exchange with untrapped electrons increases the lifetime of electron holes in inhomogeneous magnetic field. We illustrate the suggested mechanism for small-amplitude Schamel's [Phys. Scr. T2, 228–237 (1982)] electron holes and show that during propagation along a positive magnetic field gradient their amplitude should grow. Neglect of the energy exchange with untrapped electrons would result in the electron hole dissipation with only modest heating factor of trapped electrons. The suggested mechanism may contribute to generation of suprathermal electron fluxes in the space plasma.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2015

Deformation mechanism study of a hot rolled Zr-2.5Nb alloy by transmission electron microscopy. II. In situ transmission electron microscopy study of deformation mechanism change of a Zr-2.5Nb alloy upon heavy ion irradiation

The effect of heavy-ion irradiation on deformation mechanisms of a Zr-2.5Nb alloy was investigated by using the in situ transmission electron microscopy deformation technique. The gliding behavior of prismatic 〈a〉 dislocations has been dynamically observed before and after irradiation at room temperature and 300 °C. Irradiation induced loops were shown to strongly pin the gliding dislocations. Unpinning occurred while loops were incorporated into or eliminated by 〈a〉 dislocations. In the irradiated sample, loop depleted areas with a boundary parallel to the basal plane trace were found by post-mortem observation after room temperature deformation, supporting the possibility of basal channel formation in bulk neutron irradiated samples. Strong activity of pyramidal slip was also observed at both temperatures, which might be another important mechanism to induce plastic instability in irradiated zirconium alloys. Finally, (011{sup ¯}1)〈01{sup ¯}12〉 twinning was identified in the irradiated sample deformed at 300 °C.

36 MATERIALS SCIENCE↗
DOE OSTI2016

In situ electrochemical-electron spin resonance investigations of multi-electron redox reaction for organic radical cathodes

Organic radical batteries (ORBs) bearing robust radical polymers as energy storage species, are emerging promisingly with durable high energy and power characteristics by unique tunable redox properties. Here we report the development and application of in situ electrochemical-electron spin resonance (ESR) methodologies to identify the charge transfer mechanism of Poly(2,2,6,6- tetramethylpiperidinyloxy-4-yl methacrylate) (PTMA) based organic radical composite cathodes in the charge-discharge process of lithium half cells. The in situ experiments allow each electrochemical state to be associated with the chemical state (or environment) of the radical species upon the cell cycling. In situ ESR spectra of the composite cathode demonstrate a two-electron redox reaction of PTMA. Moreover, two different local environments of radical species are found in the composite electrode that includes both concentrated and isolated radicals. These two types of radicals show similarities during the redox reaction process while behave quite differently in the non-faradic reaction of ion sorption/desorption on the electrode surface.

Environmental Molecular Sciences Laboratory↗
DOE OSTI2017

Monte Carlo Simulation of Electron Thermalization in Scintillator Materials: Implications for Scintillator Nonproportionality

The lack of reliable quantitative estimates of the length and time scales associated with hot electron thermalization after a gamma-ray induced energy cascade obscures the interplay of various microscopic processes controlling scintillator performance and hampers the search for improved detector materials. We apply a detailed microscopic kinetic Monte Carlo model of the creation and subsequent thermalization of hot electrons produced by gamma irradiation of six important scintillating crystals to determine the spatial extent of the cloud of excitations produced by gamma rays and the time required for the cloud to thermalize with the host lattice. The main ingredients of the model are ensembles of microscopic track structures produced upon gamma excitation (including the energy distribution of the excited carriers), numerical estimates of electron-phonon scattering rates, and a calculated particle dispersion to relate the speed and energy of excited carriers. All these ingredients are based on first-principles density functional theory calculations of the electronic and phonon band structures of the materials. Details of the Monte Carlo model are presented along with results for thermalization time and distance distributions. These results are discussed in light of previous work. It is found that among the studied materials, calculated thermalization distances are positively correlated with measured nonproportionality. In the important class of halide scintillators, the particle dispersion is found to be more influential than the largest phonon energy in determining the thermalization distance.

Phonons, radiation detection, scintillators, thema↗
DOE OSTI2021

Processable High Electron Mobility {pi}-Copolymers via Mesoscale Backbone Conformational Ordering

The synthesis and experimental/theoretical characterization of a new series of electron-transporting copolymers based on the naphthalene bis(4,8-diamino-1,5-dicarboxyl)amide (NBA) building block are reported. Comonomers are designed to test the emergent effects of manipulating backbone torsional characteristics, and density functional theory (DFT) analysis reveals the key role of backbone conformation in optimizing electronic delocalization and transport. The NBA copolymer conformational and electronic properties are characterized using a broad array of molecular/macromolecular, thermal, optical, electrochemical, and charge transport techniques. All NBA copolymers exhibit strongly aggregated morphologies with significant nanoscale order. Copolymer charge transport properties are investigated in thin-film transistors and exhibit excellent electron mobilities ranging from 0.4 to 4.5 cm(2) V-1 s(-1). Importantly, the electron transport efficiency correlates with the film mesoscale order, which emerges from comonomer-dependent backbone planarity and extension. These results illuminate the key NBA building block structure-morphology-bulk property design relationships essential for processable, electronics-applicable high-performance polymeric semiconductors.

n‐↗
DOE OSTI2015

TiO{sub 2} nanotube arrays for photocatalysis: Effects of crystallinity, local order, and electronic structure

To furnish insight into correlations of electronic and local structure and photoactivity, arrays of short and long TiO{sub 2} nanotubes were synthesized by electrochemical anodization of Ti foil, followed by thermal treatment in O{sub 2} (oxidizing), Ar (inert), and H{sub 2} (reducing) environments. The physical and electronic structures of these nanotubes were probed with x-ray diffraction, scanning electron microscopy, and synchrotron-based x-ray absorption spectroscopy, and correlated with their photocatalytic properties. The photocatalytic activity of the nanotubes was evaluated by monitoring the degradation of methyl orange under UV-VIS light irradiation. Results show that upon annealing at 350 °C all as-anodized amorphous TiO{sub 2} nanotube samples partially transform to the anatase structure, with variations in the degree of crystallinity and in the concentration of local defects near the nanotubes' surface (∼5 nm) depending on the annealing conditions. Degradation of methyl orange was not detectable for the as-anodized TiO{sub 2} nanotubes regardless of their length. However, the annealed long nanotubes demonstrated detectable catalytic activity, which was more significant with the H{sub 2}-annealed nanotubes than with the Ar- and O{sub 2}-annealed nanotube samples. This enhanced photocatalytic response of the H{sub 2}-annealed long nanotubes relative to the other samples is positively correlated with the presence of a larger concentration of lattice defects (such as Ti{sup 3+} and anticipated oxygen vacancies) and a slightly lower degree of crystallinity near the nanotube surface. These physical and electronic structural attributes impact the efficacy of visible light absorption; moreover, the increased concentration of surface defects is postulated to promote the generation of hydroxyl radicals and thus accelerate the photodegradation of the methyl orange. The information obtained from this study provides unique insight into the role of the near-surface electronic and defect structure, crystal structure, and the local chemical environment on the photocatalytic activity and may be employed for tailoring the materials' properties for photocatalysis and other energy-related applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Compact femtosecond electron diffractometer with 100 keV electron bunches approaching the single-electron pulse duration limit

We present the design and implementation of a highly compact femtosecond electron diffractometer working at electron energies up to 100 keV. We use a multi-body particle tracing code to simulate electron bunch propagation through the setup and to calculate pulse durations at the sample position. Our simulations show that electron bunches containing few thousands of electrons per bunch are only weakly broadened by space-charge effects and their pulse duration is thus close to the one of a single-electron wavepacket. With our compact setup, we can create electron bunches containing up to 5000 electrons with a pulse duration below 100 fs on the sample. We use the diffractometer to track the energy transfer from photoexcited electrons to the lattice in a thin film of titanium. This process takes place on the timescale of few-hundred femtoseconds and a fully equilibrated state is reached within 1 ps.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2021

Exact solution of two simple non-equilibrium electron-phonon and electron-electron coupled systems: The atomic limit of the Holstein-Hubbard model and the generalized Hatsugai-Komoto model

One of the challenges in many-body physics is determining the effects of phonons on strongly correlated electrons. The difficulty arises from strong correlations at differing energy scales—for band metals, Migdal-Eliashberg theory accurately determines electron-phonon coupling effects due to the absence of vertex corrections, but strongly correlated electrons require a more complex description, and the standard Migdal-Eliashberg approach does not necessarily apply. In this work, we solve for the atomic limit Green's function of the Holstein-Hubbard model with both time-dependent electron-electron and electron-phonon couplings. Then, we examine the photoemission spectra of this model in and out of equilibrium. Next, we use similar methods to exactly solve an extended version of the Hatsugai-Komoto model and examine its behavior in and out of equilibrium. These calculations lead us to propose using the first moment of the photoemission spectra to signal non-equilibrium changes in electron-electron and electron-phonon couplings.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2017

Analysis of Multilayer Devices for Superconducting Electronics by High-Resolution Scanning Transmission Electron Microscopy and Energy Dispersive Spectroscopy

We used a focused ion beam to obtain cross-sectional specimens from both magnetic multilayer and Nb/Al-AlOx/Nb Josephson junction devices for characterization by scanning transmission electron microscopy (STEM) and energy dispersive X-ray spectroscopy (EDX). An automated multivariate statistical analysis of the EDX spectral images produced chemically unique component images of individual layers within the multilayer structures. STEM imaging elucidated distinct variations in film morphology, interface quality, and/or etch artifacts that could be correlated to magnetic and/or electrical properties measured on the same devices.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2019

Electronic and structural features of octa-coordinated yttrium–ammonia complexes: the first neutral solvated electron precursor with eight ligands and three outer electrons

The neutral and charged yttrium metal–ammonia complexes, [Y(NH3)8]0,±, are investigated using state-of-the-art quantum chemical calculations. The electronic structure of these complexes is described as an Y(NH3)83+ core with two, three, and four electrons orbiting in its periphery. Unlike the so far reported solvated electron precursors containing alkali, alkaline earth or first-row transition metals, yttrium complexes are the only ones which can accommodate eight ammonia ligands and up to four peripheral electrons. For the neutral species, two electrons occupy the diffuse s-type orbital (1s) and one diffuse p-type orbital (1p). For the cationic counterpart one electron is removed from the 1p orbital, while for the anion another electron is added to the 1p shell. The calculated low-lying electronic states with excitation energies up to 2.0 eV populate the 1s, 1p, and 1d outer orbitals. The first ionization energy of Y(NH3)8 is 2.74 eV and its electron affinity is 0.64 eV. The present results suggest that saturated yttrium ammonia solutions will turn into solids (liquid or expanded metals), where a grid of Y(NH3)83+ centers will be surrounded by “free” electrons.

Almeida, Nuno M. S.↗
DOE OSTI2023

Deep Learning Approach for High-accuracy Electron Counting of Monolithic Active Pixel Sensor-type Direct Electron Detectors at Increased Electron Dose

Abstract Electron counting can be performed algorithmically for monolithic active pixel sensor direct electron detectors to eliminate readout noise and Landau noise arising from the variability in the amount of deposited energy for each electron. Errors in existing counting algorithms include mistakenly counting a multielectron strike as a single electron event, and inaccurately locating the incident position of the electron due to lateral spread of deposited energy and dark noise. Here, we report a supervised deep learning (DL) approach based on Faster region-based convolutional neural network (R-CNN) to recognize single electron events at varying electron doses and voltages. The DL approach shows high accuracy according to the near-ideal modulation transfer function (MTF) and detector quantum efficiency for sparse images. It predicts, on average, 0.47 pixel deviation from the incident positions for 200 kV electrons versus 0.59 pixel using the conventional counting method. The DL approach also shows better robustness against coincidence loss as the electron dose increases, maintaining the MTF at half Nyquist frequency above 0.83 as the electron density increases to 0.06 e−/pixel. Thus, the DL model extends the advantages of counting analysis to higher dose rates than conventional methods.

Materials Science↗
DOE OSTI2015

Influences of Quantum Mechanically Mixed Electronic and Vibrational Pigment States in 2D Electronic Spectra of Photosynthetic Systems: Strong Electronic Coupling Cases

In 2D electronic spectroscopy studies, long-lived quantum beats have recently been observed in photosynthetic systems, and several theoretical studies have suggested that the beats are produced by quantum mechanically mixed electronic and vibrational states. Concerning the electronic-vibrational quantum mixtures, the impact of protein-induced fluctuations was examined by calculating the 2D electronic spectra of a weakly coupled dimer with the Franck-Condon active vibrational modes in the resonant condition. This analysis demonstrated that quantum mixtures of the vibronic resonance are rather robust under the influence of the fluctuations at cryogenic temperatures, whereas the mixtures are eradicated by the fluctuations at physiological temperatures. However, this conclusion cannot be generalized because the magnitude of the coupling inducing the quantum mixtures is proportional to the inter-pigment electronic coupling. In this paper, we explore the impact of the fluctuations on electronic-vibrational quantum mixtures in a strongly coupled dimer with an off-resonant vibrational mode. Toward this end, we calculate energy transfer dynamics and 2D electronic spectra of a model dimer that corresponds to the most strongly coupled bacteriochlorophyll molecules in the Fenna-Matthews-Olson complex in a numerically accurate manner. The quantum mixtures are found to be robust under the exposure of protein-induced fluctuations at cryogenic temperatures, irrespective of the resonance. At 300 K, however, the quantum mixing is disturbed more strongly by the fluctuations, and therefore, the beats in the 2D spectra become obscure even in a strongly coupled dimer with a resonant vibrational mode. Further, the overall behaviors of the energy transfer dynamics are demonstrated to be dominated by the environment and coupling between the 0 0 vibronic transitions as long as the Huang-Rhys factor of the vibrational mode is small. Finally, the electronic-vibrational quantum mixtures do not necessarily play a significant role in electronic energy transfer dynamics despite contributing to the enhancement of long-lived quantum beating in the 2D spectra.

2D electronic spectra↗