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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 415 records · Page 23
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Photocatalytic Hydrogen Evolution by a De Novo Designed Metalloprotein that Undergoes Ni–Mediated Oligomerization Shift

De novo metalloprotein design involves the construction of proteins guided by specific repeat patterns of polar and apolar residues, which, upon self-assembly, provide a suitable environment to bind metals and produce artificial metalloenzymes. While a wide range of functionalities have been realized in de novo designed metalloproteins, the functional repertoire of such constructs towards alternative energy-relevant catalysis is currently limited. Here we show the application of de novo approach to design a functional H 2 evolving protein. The design involved the assembly of an amphiphilic peptide featuring cysteines at tandem a/d sites of each helix. Intriguingly, upon Ni II addition, the oligomers shift from a major trimeric assembly to a mix of dimers and trimers. The metalloprotein produced H 2 photocatalytically with a bell-shape pH dependence, having a maximum activity at pH 5.5. Transient absorption spectroscopy is used to determine the timescales of electron transfer as a function of pH. Selective outer sphere mutations are made to probe how the local environment tunes activity. Finally, a preferential enhancement of activity is observed via steric modulation above the Ni II site, towards the N-termini, compared to below the Ni II site towards the C-termini.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Characterization of injection and confinement improvement through impurity induced profile modifications on the Wendelstein 7-X stellarator

Pulsed injections of boron carbide granules into Wendelstein 7-X stellarator (W7-X) plasmas transiently increase the plasma stored energy and core ion temperatures above the reference W7-X experimental programs by up to 30%. In a series of 4 MW electron cyclotron resonance heating experiments, the PPPL Probe Mounted Powder Injector provided 50 ms bursts of 100 μm granules every 350 ms at estimated quantities ranging from approximately 1 mg/pulse to over 30 mg/pulse. For each injection, the stored energy was observed to initially drop and the radiated power transiently increased, while the radial electron density profile rose at the edge as material was assimilated. Once the injected boron carbide was fully absorbed, the density rise transitioned to the core while the stored energy increased above the previous baseline level by an amount linearly correlated with the injection quantity. During the injection, the ion temperature gradient steepened with peak core ion temperatures observed to increase from a nominal 1.7 keV to over 2.6 keV for the largest injection amounts. Enhanced performance is accompanied by a reversal of the radial electric field at ρ < 0.3, indicating that the core transport has switched to the ion root. These observations are suggestive of a change in transport and provide further evidence that externally induced profile modifications provide a possible path to enhanced W7-X performance metrics.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2024

Single-Molecule Detection of the Encounter and Productive Electron Transfer Complexes of a Photosynthetic Reaction Center

Small, diffusible redox proteins play an essential role in electron transfer (ET) in respiration and photosynthesis, sustaining life on Earth by shuttling electrons between membrane-bound complexes via finely tuned and reversible interactions. Ensemble kinetic studies show transient ET complexes form in two distinct stages: an “encounter” complex largely mediated by electrostatic interactions, which subsequently, through subtle reorganization of the binding interface, forms a “productive” ET complex stabilized by additional hydrophobic interactions around the redox-active cofactors. Here, using single-molecule force spectroscopy (SMFS) we dissected the transient ET complexes formed between the photosynthetic reaction center-light harvesting complex 1 (RC-LH1) of Rhodobacter sphaeroides and its native electron donor cytochrome c 2 (cyt c 2 ). Importantly, SMFS resolves the distribution of interaction forces into low (~150 pN) and high (~330 pN) components, with the former more susceptible to salt concentration and to alteration of key charged residues on the RC. Thus, the low force component is suggested to reflect the contribution of electrostatic interactions in forming the initial encounter complex, whereas the high force component reflects the additional stabilization provided by hydrophobic interactions to the productive ET complex. Employing molecular dynamics simulations, we resolve five intermediate states that comprise the encounter, productive ET and leaving complexes, predicting a weak interaction between cyt c 2 and the LH1 ring near the RC-L subunit that could lie along the exit path for oxidized cyt c 2 . The multimodal nature of the interactions of ET complexes captured here may have wider implications for ET in all domains of life.

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

Electronic Tuning of Photoexcited Dynamics in Heteroleptic Cu(I) Complex Photosensitizers

Photoexcited dynamics of heteroleptic Cu(I) complexes as noble-metal-free photosensitizers are closely intertwined with the nature of their ligands. By utilizing ultrafast optical and X-ray transient absorption spectroscopies, we characterized a new set of heteroleptic Cu(I) complexes [Cu(PPh 3 )( 2 )(BPy R )] + (R = CH 3 , H, Br to COOCH 3 ), with an increase in the electron-withdrawing ability of the functional group (R). Here we found that after the transient photooxidation of Cu(I) to Cu(II), the increasing electron-withdrawing ability of R barely affects the internal conversion (IC) (e.g., Jahn-taller (JT) distortion) between singlet MLCT states. However, it does accelerate the dynamics of intersystem crossing (ISC) between singlet and triplet MLCT states and the subsequent decay from the triplet MLCT state to the ground state. The associated lifetime constants are reduced by up to 300%. Our understanding of the photoexcited dynamics in heteroleptic Cu(I) complexes through ligand electronic tuning provides valuable insight into the rational design of efficient Cu(I) complex photosensitizers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2001

Synchronized Electronic Shutter System (SESS) for Thermal Nondestructive Evaluation

The purpose of this paper is to describe a new method for thermal nondestructive evaluation. This method uses a synchronized electronic shutter system (SESS) to remove the heat lamp's influence on the thermal data during and after flash heating. There are two main concerns when using flash heating. The first concern is during the flash when the photons are reflected back into the camera. This tends to saturate the detectors and potentially introduces unknown and uncorrectable errors when curve fitting the data to a model. To address this, an electronically controlled shutter was placed over the infrared camera lens. Before firing the flash lamps, the shutter is opened to acquire the necessary background data for offset calibration. During flash heating, the shutter is closed to prevent the photons from the high intensity flash from saturating the camera's detectors. The second concern is after the flash heating where the lamps radiate heat after firing. This residual cooling introduces an unwanted transient thermal response into the data. To remove this residual effect, a shutter was placed over the flash lamps to block the infrared heat radiating from the flash head after heating. This helped to remove the transient contribution of the flash. The flash lamp shutters were synchronized electronically with the camera shutter. Results are given comparing the use of the thermal inspection with and without the shutter system.

Zalameda, Joseph N.↗
NASA NTRS2006

The Dissipation Mechanism in Collisionless Magnetic Reconnection

The dissipation mechanism of magnetic reconnection remains a subject of intense scientific interest. On one hand, one set of recent studies have shown that particle inertia-based processes, which include thermal and bulk inertial effects, provide the reconnection electric field in the diffusion region. On the other hand, a second set of studies emphasizes the role of wave-particle interactions in providing anomalous resistivity in the diffusion region. In this presentation, we present analytical theory results, as well as PIC simulations of guide-field magnetic reconnection. We will show that the thermal electron inertia-based dissipation mechanism, expressed through nongyrotropic electron pressure tensors, remains viable in three dimensions. We will demonstrate the thermal inertia effect through studies of electron distribution functions. Furthermore, we will show that the reconnection electric field provides a transient acceleration on particles traversing the inner reconnection region. This inertial effect can be described as a diffusion-like term of the current density, which matches key features of electron distribution functions.

Hesse, Michael↗
NASA NTRS2008

The Electron Diffusion Region: Forces and Currents

The dissipation mechanism of magnetic reconnection remains a subject of intense scientific interest. On one hand, one set of recent studies have shown that particle inertia-based processes, which include thermal and bulk inertial effects, provide the reconnection electric field in the diffusion region. On the other hand, a second set of studies emphasizes the role of wave-particle interactions in providing anomalous resistivity in the diffusion region. In this presentation, we present analytical theory results, as well as PIC simulations of guide-field magnetic reconnection. We will show that the thermal electron inertia-based dissipation mechanism, expressed through nongyrotropic electron pressure tensors, remains viable in three dimensions. We will demonstrate the thermal inertia effect through studies of electron distribution functions. Furthermore, we will show that the reconnection electric field provides a transient acceleration on particles traversing the inner reconnection region. This inertia1 effect can be described as a diffusion-like term of the current density, which matches key features of electron distribution functions.

Hesse, Michael↗
NASA NTRS2009

What Turns Reconnection On and Off

The dissipation mechanism of magnetic reconnection remains a subject of intense scientific interest. On one hand, one set of recent studies have shown that particle inertia-based processes, which include thermal and bulk inertial effects, provide the reconnection electric field in the diffusion region. On the other hand, a second set of studies emphasizes the role of wave-particle interactions in providing anomalous resistivity in the diffusion region. In this presentation, we present analytical theory results, as well as PIC simulations of guide-field magnetic reconnection. We will show that the thermal electron inertia-based dissipation mechanism, expressed through nongyrotropic electron pressure tensors, remains viable in three dimensions. We will demonstrate the thermal inertia effect through studies of electron distribution functions. Furthermore, we will show that the reconnection electric field provides a transient acceleration on particles traversing the inner reconnection region. This inertial effect can be described as a diffusion-like term of the current density. which matches key features of electron distribution functions.

Hesse, Michael↗
NASA NTRS2009

The Electron Diffusion Region: Forces and Currents

The dissipation mechanism of magnetic reconnection remains a subject of intense scientific interest. On one hand, one set of recent studies have shown that particle inertia-based processes, which include thermal and bulk inertial effects, provide the reconnection electric field in the diffusion region. On the other hand, a second set of studies emphasizes the role of wave-particle interactions in providing anomalous resistivity in the diffusion region. In this presentation, we present analytical theory results, as well as PIC simulations of guide-field magnetic reconnection. We will show that the thermal electron inertia-based dissipation mechanism, expressed through nongyrotropic electron pressure tensors, remains viable in three dimensions. We will demonstrate the thermal inertia effect through studies of electron distribution functions. Furthermore, we will show that the reconnection electric field provides a transient acceleration on particles traversing the inner reconnection region. This inertial effect can be described as a diffusion-like term of the current density, which matches key features of electron distribution functions.

Hesse, Michael↗
DOE OSTI2022

Nonequilibrium Lattice Dynamics in Photoexcited 2D Perovskites

Abstract Interplay between structural and photophysical properties of metal halide perovskites is critical to their utility in optoelectronics, but there is limited understanding of lattice response upon photoexcitation. Here, 2D perovskites butylammonium lead iodide, (BA) 2 PbI 4 , and phenethylammonium lead iodide, (PEA) 2 PbI 4 , are investigated using ultrafast transient X‐ray diffraction as a function of optical excitation fluence to discern structural dynamics. Both powder X‐ray diffraction and time‐resolved photoluminescence linewidths narrow over 1 ns following optical excitation for the fluence range studied, concurrent with slight redshifting of the optical bandgaps. These observations are attributed to transient relaxation and ordering of distorted lead iodide octahedra stimulated mainly by electron–hole pair creation. The c axis expands up to 0.37% over hundreds of picoseconds; reflections sampling the a and b axes undergo one tenth of this expansion with the same timescale. Post‐photoexcitation appearance of the (110) reflection in (BA) 2 PbI 4 would suggest a transient phase transition, however, through new single‐crystal XRD, reflections are found that violate glide plane conditions in the reported Pbca structure. The static structure space group is reassigned as P 2 1 2 1 2 1 . With this, a nonequilibrium phase transition is ruled out. These findings offer increased understanding of remarkable lattice response in 2D perovskites upon excitation.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Extreme ultraviolet transient gratings: A tool for nanoscale photoacoustics

Collective lattice dynamics determine essential aspects of condensed matter, such as elastic and thermal properties. These exhibit strong dependence on the length-scale, reflecting the marked wavevector dependence of lattice excitations. The extreme ultraviolet transient grating (EUV TG) approach has demonstrated the potential of accessing a wavevector range corresponding to the 10s of nm length-scale, representing a spatial scale of the highest relevance for fundamental physics and forefront technology, previously inaccessible by optical TG and other inelastic scattering methods. In this manuscript we report on the capabilities of this technique in the context of probing thermoelastic properties of matter, both in the bulk and at the surface, as well as discussing future developments and practical considerations.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

High-resolution radiation detection using Ni/SiO 2 /n-4H-SiC vertical metal-oxide-semiconductor capacitor

In this article, we demonstrate the radiation detection performance of vertical metal-oxide-semiconductor (MOS) capacitors fabricated on 20 μm thick n-4H-SiC epitaxial layers with the highest energy resolution ever reported. The 100 nm SiO2 layer was achieved on the Si face of n-4H-SiC epilayers using dry oxidation in air. The Ni/SiO2/n-4H-SiC MOS detectors not only demonstrated an excellent energy resolution of 0.42% (ΔE/E 100) for 5.48 MeV alpha particles but also caused a lower enhancement in the electronic noise components of the spectrometer compared with that observed for the best high-resolution Schottky barrier detectors. The MOS detectors also exhibited a high charge collection efficiency (CCE) of 96% at the optimized operating bias despite the presence of the oxide layer. A drift-diffusion model applied to the CCE vs gate bias voltage data revealed a minority (hole) carrier diffusion length of 24 μm. Capacitance mode deep level transient spectroscopy (C-DLTS) scans in the temperature range 84–800 K were carried out to identify the resolution limiting electrically active defects. Interestingly, the C-DLTS spectra revealed both positive and negative peaks, indicating the simultaneous presence of electron (majority) and hole (minority) trap centers. It has been inferred that at the steady-state bias for the C-DLTS measurement, the MOS detector operates in the inversion mode at certain device temperatures, causing holes to populate the minority trap centers and, hence, manifests minority carrier peaks as well.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
NASA NTRS1973

The chromospheric association of the metric type 3 bursts - implications concerning the acceleration of solar electrons and the active streamers

In two recent papers it was shown that the metric type 3 emission is closely related to a transient perturbation seen in absorption in the H alpha line. In addition, this perturbation sometimes triggers a flare, sometimes not. This can explain why the type 3 have a poor H alpha flare correlation rate and still are a typical flash phase emission when flare-associated. The characteristics are summarized of the new association proposed. It is assumed that 10 to 100 keV electrons are accelerated in connection with a particular kind of transient H alpha absorbing feature. For as yet undetermined reasons, this process would often, but not always, result in a more efficient acceleration coincident with the early phase of the optical flare. The possibilities that this process could lead occasionally to long lasting subrelativistic particle emissive region are explored.

Axisa, F.↗
DOE OSTI2024

Attosecond delays in X-ray molecular ionization

The photoelectric effect is not truly instantaneous, but exhibits attosecond delays that can reveal complex molecular dynamics. Sub-femtosecond duration light pulses provide the requisite tools to resolve the dynamics of photoionization. Accordingly, the past decade has produced a large volume of work on photoionization delays following single photon absorption of an extreme ultraviolet (XUV) photon. However, the measurement of time-resolved core-level photoionization remained out of reach. The required x-ray photon energies needed for core-level photoionization were not available with attosecond tabletop sources. We have now measured the x-ray photoemission delay of core-level electrons, and here report unexpectedly large delays, ranging up to 700 attoseconds in NO near the oxygen K-shell threshold. These measurements exploit attosecond soft x-ray pulses from a free-electron laser (XFEL) to scan across the entire region near the K-shell threshold. Furthermore, we find the delay spectrum is richly modulated, suggesting several contributions including transient trapping of the photoelectron due to shape resonances, collisions with the Auger-Meitner electron that is emitted in the rapid non-radiative relaxation of the molecule, and multi-electron scattering effects. Finally, the results demonstrate how x-ray attosecond experiments, supported by comprehensive theoretical modelling, can unravel the complex correlated dynamics of core-level photoionization.

74 ATOMIC AND MOLECULAR PHYSICS↗
NASA NTRS1985

DLTS analysis of radiation-induced defects in one-MeV electron irradiated germanium and Alsub0.17Gasub0.83As solar cells

The radiation-induced deep-level defects in one-MeV electron-irradiated germanium and AlxGal-xAs solar cell materials using the deep-level transient spectroscopy (DLTS) and C-V techniques were investigated. Defect and recombination parameters such as defect density and energy levels, capture cross sections and lifetimes for both electron and hole traps were determined. The germanium and AlGaAs p/n junction cells were irradiated by one-MeV electrons. The DLTS, I-V, and C-V measurements were performed on these cells. The results are summarized as follows: (1) for the irradiated germanium samples, the dominant electron trap was due to the E sub - 0.24 eV level with density around 4x10 to the 14th power 1/cu cm, independent of electron fluence, its origin is attributed to the vacancy-donor complex defect formed during the electron irradiation; (2) in the one-MeV electron irradiated Al0.17Ga0.83 as sample, two dominant electron traps with energies of Ec-0.19 and -0.29 eV were observed, the density for both electron traps remained nearly constant, independent of electron fluence. It is shown that one-MeV electron irradiation creates very few or no new deep-level traps in both the germanium and AlxGa1-xAs cells, and are suitable for fabricating the radiation-hard high efficiency multijunction solar cells for space applications.

Li, S. B.↗
DOE OSTI2021

Integrated transmission electron microscope

An integrated transmission electron microscope comprising multiple electron sources for tuned beams of ultrafast, scanning probe, and parallel illumination in varied beam energies can be alternated within sub-microseconds onto a sample with dynamic ‘transient state’ processes to acquire atomic-scale structural/chemical data with site specificity. The various electron sources and condenser optics enable high-resolution imaging, high-temporal resolution imaging, and chemical imaging, using fast-switching magnets to direct the different electron beams onto a single maneuverable objective pole piece where the sample resides. Such multimodal in situ characterization tools housed in a single microscope have the potential to revolutionize materials science.

Jungjohann, Katherine L.↗
NASA NTRS1990

Femtosecond optical absorption studies of nonequilibrium electronic processes in high T(c) superconductors

The results are reported of femtosecond optical transient absorption experiments performed on the superconducting compounds YBa2Cu3O(7-x) (x about 0) and Bi2Sr2Ca2Cu3O(10+delta) (delta about 0) and nonsuperconducting YBa2Cu3O(6+y) (y less than 0.4) for sample temperatures ranging from about 7 K to room temperature. Nonequilibrium heating was found to occur on a subpicosecond time scale. A distinct, dramatic increase in the relaxation time was observed for the superconducting samples as the sample temperature was lowered below the critical temperatures of the respective films. Accompanying the increase in relaxation time was an increase in the peak fractional transmissivity change. No such changes were observed for the nonsuperconducting YBCO sample.

Chwalek, J. M.↗