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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 73 records · Page 4
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Electrical control of spin relaxation anisotropy during drift transport in a two-dimensional electron gas

Spin relaxation was studied in a two-dimensional electron gas confined in a wide GaAs quantum well. Recently, the control of the spin relaxation anisotropy by diffusive motion was first shown in D. Iizasa et al., arXiv:2006.08253. Here, we demonstrate electrical control by drift transport in a system with two subbands occupied. The combined effect of in-plane and gate voltages was investigated using time-resolved Kerr rotation. Furthermore, the measured relaxation time presents strong anisotropy with respect to the transport direction. For an in-plane accelerating electric field along [110], the lifetime was strongly suppressed irrespective of the applied gate voltage. Remarkably, for transport along [$1\bara{1}0$], the data shows spin lifetime that was gate dependent and longer than in the [110] direction regardless of the in-plane voltage. In agreement, independent results of anisotropic spin precession frequencies are also presented. Nevertheless, the long spin lifetime, strong anisotropy and drift response seen in the data are beyond the existing models for spin drift and diffusion.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Quantum efficiency, photoemission energy spectra, and mean transverse energy of ultrananocrystalline diamond photocathode

The quantum efficiency and mean transverse energy of electrons emitted from a cathode determine the quality of beams generated from photoinjectors. The nitrogen-incorporated ultrananocrystalline diamond, (N)UNCD, is a new class of robust semiconductor photocathodes, which has been considered in photoinjectors for high peak current extraction. In this work, we measure the spectral response in quantum efficiency, photoemission energy spectra, and mean transverse energy of the (N)UNCD photocathode using a photoemission electron microscope. The observed quantum efficiency was comparable to that of copper photocathodes. Photoemission spectra showed the evidence of scattering of electrons before emission. This relaxation of electrons due to scattering is also observed in the spectral response of the mean transverse energy. The mean transverse energy is limited to ∼70 meV at the threshold. We attribute this to the physical and chemical roughness of the (N)UNCD photocathode and, hence, smoother films will be required to further reduce the mean transverse energy obtained from the (N)UNCD photocathode.

Kachwala, A. (ORCID:0000000301756478)↗
DOE OSTI2021

Electron Kinetics Induced by Ultrafast Photoexcitation of Warm Dense Matter in a 30-nm-Thick Foil

We report on the study of electron kinetics induced by intense femtosecond (fs) laser excitation of electrons in the 5d band of Au. Changes in the electron system are observed from the temporal evolution of ac conductivity and conduction electron density. The results reveal an increase of electron thermalization time with excitation energy density, contrary to the Fermi-liquid behavior of the decrease of thermalization time associated with the heating of conduction electrons. This is attributed to the severe mitigation of photoexcitation by Auger decay. The study also uncovers the shortening of 5d hole lifetime with the increase of photoexcitation rates. Overall, these unique findings provide valuable insights for understanding electron kinetics under extreme nonequilibrium conditions.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2024

Nanometer-Scale Acoustic Wave Packets Generated by Stochastic Core-Level Photoionization Events

We demonstrate that the absorption of femtosecond hard x-ray pulses excites quasispherical, high-amplitude, and high-wave-vector coherent acoustic phonon wave packets using an all hard-x-ray pump-probe scattering experiment. The time- and momentum-resolved diffuse scattering signal is consistent with an ensemble of 3D strain wave packets induced by the rapid electron cascade dynamics following photoionization at uncorrelated excitation centers. We quantify key parameters of this process, including the localization size of the stress field and the photon energy conversion efficiency into elastic energy. The parameters are determined by the photoelectron and Auger electron cascade dynamics, as well as the electron-phonon interaction. In particular, we obtain the localization size of the observed strain wave packet to be 1.5 and 2.5 nm for bulk SrTiO 3 and KTaO 3 single crystals, respectively. The results provide crucial information on the mechanism of x-ray energy deposition into matter and shed light on the shortest collective length scales accessible to coherent acoustic phonon generation using x-ray excitation. Published by the American Physical Society 2024

36 MATERIALS SCIENCE↗
DOE OSTI2020

Magnetic anomalies associated with domain wall freezing and coupled electron hopping in magnetite nanorods

Magnetite has fascinated researchers for decades, due to its wide range of applications from spintronics to biomedicine. Despite a large body of works aimed at its magnetic properties, no consensus has been reached on the physical origin of the low temperature magnetic anomalies observed in magnetite. Although, a lot of work has been done in studying magnetite nanoparticles, but studies on the low temperature anomalies in those nanoparticles still remains unresearched. We report on the observation of the low temperature magnetic anomalies in highly crystalline, stoichiometric Fe 3 O 4 nanorods and relate them to the coupled electron hopping relaxation process and domain wall motion. Both DC and AC susceptibility show the presence of a hump around 35 K, which is associated with the relaxation of Fe +2 extra electrons. Radiofrequency transverse susceptibility (TS) measurements indicated a noticeable increase in anisotropy field below ~ 25 K, which is attributed to the rearrangement of Fe +2 electrons in the octahedral sites. TS experiments also revealed the domain wall freezing below ~35 K. Our combined DC, AC and TS susceptibility studies shed light on the complex nature of the lowtemperature magnetic behavior in nanostructured magnetite.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Mechanistic implications of excited high-spin states, spin–spin coupling, and differential [2Fe–2S] + cluster temperature relaxations in the electron-bifurcating NfnABC from Thermococcus sibiricus

Electron bifurcation (EB) is a mechanism of biological energy transduction in which multiple oxidation–reduction (redox) reactions are thermodynamically coupled within a single enzyme, enabling the enzyme to harness the excess free energy from an exergonic process to drive an endergonic process. Because of this unprecedented chemistry, there is interest to translate EB principles to artificial and bioengineered systems, but a hurdle is that knowledge pertaining to the fundamental design principles of EB enzymes remains scarce. Here, we investigated the fundamental physical and electronic properties of electron transfer sites in a spectroscopically uncharacterized member of the BfuABC family of EB enzymes, the NADH-dependent reduced-ferredoxin:NADP + oxidoreductase from Thermococcus sibiricus (Tsi NfnABC). Cryo-EM structures of Tsi NfnABC previously demonstrated that it contains twelve redox cofactors: two flavins (one FAD and one FMN), eight [4Fe–4S] clusters, and two [2Fe–2S] clusters. The FMN, one [4Fe–4S] cluster, and one [2Fe–2S] cluster comprise the bifurcating active site termed the electron-bifurcating flavobicluster (BF-FBC), which is found in all BfuABC family members. By using electron paramagnetic resonance spectroscopy, we identified spectral signatures originating from interactions between the FMN radical and [4Fe–4S] + cluster in the BF-FBC and observed temperature dependent behavior of the BF-FBC's [2Fe–2S] + cluster indicative of moderately slow spin–lattice relaxation. Additionally, we uncovered numerous spectral features corresponding to half-integer, S > ½ spin states of [4Fe–4S] + clusters, including one attributable to the consequences of lysine-ligation of a [4Fe–4S] cluster unique to NfnABC. We contextualize these findings to electron transfer theory and NfnABC's structure. Our insights further the understanding of how enzymes are designed to exert control over electron transfer to conduct thermodynamically challenging reactions.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2021

Dynamics and chemical mode analysis of plasma thermal-chemical instability

The stability of the weakly ionized plasma and the transition from a stable homogeneous discharge to unstable filaments play an important role in gas laser physics, plasma-assisted combustion, chemical reforming, and material synthesis. Here, theoretical stability analysis and thermal-chemical mode analysis were performed to understand the mechanism of plasma thermal-chemical instability by using a zero-dimensional plasma system with both simplified and detailed chemical kinetics of H 2 /O 2 /N 2 mixtures. The plasma dynamic and kinetic models accounted for multiple physical mechanisms in the chemically-reactive weakly ionized plasma, including ionization, attachment/detachment, recombination, vibrational and electronic energy relaxation, convective and diffusive species/heat removal, Joule heating, and detailed chemical kinetics. An analytical criterion and the explosive mode species/temperature pointers were formulated while the representative active species were identified for different thermal-chemical modes. The results showed that in addition to the classical thermal-ionization mechanism, various chemical modes from chemical heat imbalance and elementary kinetics significantly modified the time dynamics and the stability of the weakly ionized plasma. The present analysis provides insights and guidance to control plasma instability using chemical kinetics.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Collective excitations and quantum incompressibility in electron-hole bilayers

In this study, we apply quantum continuum mechanics to the calculation of the excitation spectrum of a coupled electron-hole bilayer. The theory expresses excitation energies in terms of ground-state intra- and interlayer pair correlation functions, which are available from quantum Monte Carlo calculations. The final formulas for the collective modes deduced from this approach coincide with the formulas obtained in the “quasilocalized particle approximation” by Kalman et al. [G. Kalman, V. Valtchinov, and K. I. Golden, Phys. Rev. Lett. 82 , 3124 (1999) ], and likewise the theory predicts the existence of gapped excitations in the charged channel, with the gap arising from electron-hole correlation. An immediate consequence of the gap is that the static density-density response function of the charged channel vanishes as q 2 for wave vector q → 0 , rather than linearly in q , as commonly expected. In this sense, the system is incompressible . This feature, which has no analog in the classical electron-hole plasma, is consistent with the existence of an excitonic ground state and implies the existence of a discontinuity in the chemical potential of electrons and holes when the numbers of electrons and holes are equal. It should be experimentally observable by monitoring the densities of electrons and holes in response to potentials that attempt to change these densities in opposite directions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Relaxation timescales and electron-phonon coupling in optically pumped $\mathrm{YBa_2Cu_3O_{6+\mathcal{x}}}$ revealed by time-resolved Raman scattering

Time-resolved measurements provide a new way to disentangle complex interactions in quantum materials due to their different timescales. We used pump-probe Raman scattering to investigate the apical oxygen vibration in $\mathrm{YBa_2Cu_3O_{6+\mathcal{x}}}$ under nonequilibrium conditions. Time dependence of the phonon population demonstrated strong electron-phonon coupling. Most importantly, the phonon shifts to a higher energy due to transient smearing of the Fermi surface in a remarkable agreement with diagrammatic theory. Here we also discuss insights into photoinduced superconductivity reported at lower doping that follow from these results.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Plasmon Dynamics Driven by Aggregation of Tris(2,2′-bipyridine)ruthenium(II)-Functionalized Gold Nanoparticles Probed by XANES and Transient Absorption Spectroscopy

Energy conversion dynamics is critical for advancing next-generation photovoltaics, optoelectronics, and light-harvesting technologies. Noble metal plasmonic nanoparticles play a pivotal role as nanoscale electromagnetic confinement structures, driving photon-induced chemical reactions. In this study, we explore the effects of [Ru(bpy) 3 ] 2+ functionalization and aggregation on citrate-capped gold nanoparticles (AuNPs) of 40 and 100 nm diameters, focusing on molecule-plasmon interactions and their influence on electronic and energy dissipation properties. X-ray absorption near-edge spectroscopy (XANES) revealed that [Ru(bpy) 3 ] 2+ functionalization induces controlled aggregation without altering the oxidation state of gold. A more pronounced white-line intensity is observed in 40 nm AuNPs, consistent with greater s–p–d hybridization and a higher density of surface states, likely influenced by both nanoparticle size and aggregation. Transient absorption (TA) spectroscopy highlights faster electron–phonon relaxation dynamics in aggregated 40 nm nanoparticles, which is attributed to increased electron delocalization and more efficient coupling to the phonon bath. In contrast, 100 nm nanoparticles exhibit minimal changes due to a lower degree of aggregation. Interestingly, we observe that enhanced electron–phonon coupling in aggregated nanoparticles coincides with a slowing of electron–electron scattering. These observations suggest a competitive interplay between the two relaxation pathways, where enhanced energy transfer to the lattice in aggregated systems can suppress electronic thermalization. In conclusion, these findings underscore the critical role of nanoparticle size, aggregation, and molecule–surface interactions in modulating plasmonic dynamics and excited-state lifetimes and further provide valuable insights into designing tailored plasmonic systems with transformative potential for sensing, catalysis, and energy conversion.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Defect in diamond with millisecond-scale spin relaxation time at room temperature

Spin defects in diamond are promising platforms for quantum sensing. The longest electron spin relaxation times (T1) at room temperature for solid-state defects are observed in nitrogen vacancy centers in diamond, which can reach 6.67 ms [1], and substitutional nitrogen (“P1 centers”) in diamond, which exhibit a T1 of 2 ms [2]. No other solid-state defect has exhibited millisecond-scale spin relaxation times at room temperature thus far. Here, we characterize the spin properties of the WAR5 defect in diamond [3] with pulsed electron spin resonance. The observed T1 is one of the longest for solid-state spin defects: 0.97(27) ms at room temperature and 14.38(19) min at 4 K. The observed coherence time (T2) is 246(7) µs, which can be extended to 6.49(34) ms at 4 K with dynamical decoupling. Finally, we demonstrate optical spin polarization with a range of wavelengths from 405 nm to 500 nm and propose potential zero-phonon line candidates.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Dynamic pair-breaking current, critical superfluid velocity, and nonlinear electromagnetic response of nonequilibrium superconductors

Here, we report numerical calculations of a dynamic pair-breaking current density $J_d$ and a critical superfluid velocity $v_d$ in a nonequilibrium superconductor carrying a uniform, large-amplitude AC current density $J(t) = J_a$sinΩ$\textit{t}$ with Ω well below the gap frequency Ω $\ll Δ_0/ℏ$. The dependencies $J_d$(Ω, $\textit{T}$) and $v_d$(Ω, $\textit{T}$) near the critical temperature $T_c$ were calculated from either the full time-dependent nonequilibrium equations for a dirty $\textit{s}$-wave superconductor or the time-dependent Ginzburg-Landau (TDGL) equations for a gapped superconductor, taking into account the GL relaxation time of the order parameter $τ_{\text{GL}}$ and the inelastic electron-phonon relaxation time of quasiparticles $τ_E$. We show that both approaches give similar frequency dependencies of $J_d$(Ω) and $v_d$(Ω) which gradually increase from their static pair-breaking GL values $J_c$ and $v_c$ at Ω$τ_E \ll$1 to $\sqrt{2}J_c$ and $\sqrt{2}v_c$ at Ω$τ_E \gg$ 1. Here $J_d, v_d$ and a dynamic superheating field at which the Meissner state becomes unstable were calculated in two different regimes of a fixed AC current and a fixed AC superfluid velocity induced by the applied AC magnetic field $H = H_a$ sinΩ$\textit{t}$ in a thin superconducting filament or a type-II superconductor with a large GL parameter. We also calculated a nonlinear electromagnetic response of a nonequilibrium superconducting state, particularly a dynamic kinetic inductance and a dissipative quasiparticle conductivity, taking into account the oscillatory dynamics of superconducting condensate and the kinetics of quasiparticles driven by a strong AC current. It is shown that an AC current density produces multiple harmonics of the electric field, the amplitudes of the higher-order harmonics diminishing as $τ_E$ increases.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Measurements of Electron Beam-Induced Spin-Relaxation in Frozen-Spin Hydrogen-Deuteride (HD)

Targets of solid hydrogen-deuteride (HD) can be prepared in a frozen-spin state with spin relaxation times (T1) in excess of a year. The present work has studied their potential use in experiments with electron beams. Polarization relaxation rates have been measured during exposure to sub-nanoAmp currents of 9.7 MeV electron beams from the recently commissioned Upgraded Injector Test Facility (UITF) at Jefferson Lab (JLab). These UITF measurements can be used to anticipate the expected performance at the GeV energies typical of JLab experiments, since the energy deposition in a target is almost independent of beam energy. An in-beam dilution refrigerator equipped with superconducting solenoids has been used to maintain solid HD samples at ?0.1 K and ?1 tesla, and internal NMR coils have been used to monitor hydrogen polarization. Spin-relaxation in two frozen-spin targets, with initial H-polarizations of 40% and 34%, have been tracked while exposed to beams under varying conditions of current, dose, beam duty factor and temperature. At a fixed accumulated dose, the spin-relaxation rates drop with current, suggesting depolarization by the charge cloud of the beam. Imposing a duty factor on the otherwise continuous UITF beam, with forced millisecond scale gaps, has shown no obvious correlation to polarization loss rates. After an accumulated dose of ?2 ?C/cm2, beam-off spin-relaxation rates drop from their immeasurably long pre-irradiation values to the order of weeks (with beam-on T1 values typically an order of magnitude shorter), reflecting a buildup of paramagnetic charge centers within the HD lattice. The accumulated polarization loss was approximately proportional to dose in both targets, dropping to 1/e of their initial values after ?6 ?C/cm2. Thermal equilibrium polarizations of targets not in the frozen-spin state (with intentionally short T1) have been used to deduce the in situ temperature of solid HD while under electron bombardment. A model for depolarization by beam-associated paramagnetic impurities largely accounts for the data, and suggests that improvements in heat removal could lead to significant increases in the in-beam T1.

O'Connell, Thomas↗
DOE OSTI2021

Resonant two-photon photoelectron imaging and adiabatic detachment processes from bound vibrational levels of dipole-bound states

Anions cannot have Rydberg states, but anions with polar neutral cores can support highly diffuse dipole-bound states (DBSs) as a class of interesting electronically excited states below the electron detachment threshold. The binding energies of DBSs are extremely small, ranging from a few to few hundred wavenumbers and generally cannot support bound vibrational levels below the detachment threshold. Thus, vibrational excitations in the DBS are usually above the electron detachment threshold and they have been used to conduct resonant photoelectron spectroscopy, which is dominated by state-specific autodetachment. Here we report an investigation of a cryogenically-cooled complex anion, the enantiopure (R)-(–)-1-(9-anthryl)-2,2,2-trifluoroethanolate (R-TFAE–). The neutral R-TFAE radical is relatively complex and highly polar with a non-planar structure (C 1 symmetry). Photodetachment spectroscopy reveals a DBS 209 cm–1 below the detachment threshold of R-TFAE– and seven bound and eight above-threshold vibrational levels of the DBS. Resonant two-photon detachment (R2PD) via the bound vibrational levels of the DBS exhibits strictly adiabatic photodetachment behaviors by the second photon, in which the vibrational energies in the DBS are carried to the neutral final states, because of the parallel potential energy surfaces of the DBS and the corresponding neutral ground electronic state. Relaxation processes from the bound DBS levels to the ground and low-lying electronically excited states of R-TFAE– are also observed in the R2PD photoelectron spectra. Finally, the combination of photodetachment and resonant photoelectron spectroscopy yields frequencies for eight vibrational modes of the R-TFAE radical.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Theoretical and global simulation analysis of collisional microtearing modes

Microtearing modes (MTMs) are suggested as a candidate for anomalous thermal transport in tokamak H-mode discharges. This study investigates MTMs in tokamak plasmas, employing simulations in the BOUT++ framework. It simplifies and linearizes the governing equations in detailed linear simulations. The study meticulously evaluates various conductivity models under diverse plasma conditions and collision regimes. The research thoroughly assesses different conductivity models across a range of plasma conditions and collision regimes. A unified dispersion relation that includes both MTM and Drift-Alfvén Wave (DAW) instabilities is derived, showing that DAW and MTM instabilities occur at varying distances from the rational surface. Specifically, MTMs become unstable near the rational surface but stabilize farther away, while drift-Alfvén instability appears farther from the rational surface. The study also re-derives MTM dispersion relations using Ohm's law and the vorticity equation, providing a thorough analysis of electromagnetic and electrostatic interactions in tokamaks. Global simulations demonstrate an inverse correlation between MTM growth rates and collisionality, and a direct correlation with temperature gradients. The nonalignment of the rational surface with the peak ω*e stabilizes the MTMs. Nonlinear simulations highlight electron temperature relaxation as the primary saturation mechanism for MTMs, with magnetic flutter identified as the dominant mode of electron thermal transport.

Fan, K. (ORCID:0000000227518809)↗
DOE OSTI2025

Trap-assisted Auger-Meitner recombination in GaN p-i-n diodes

Most properties of semiconductor devices are dominated by shallow impurities. However, deep defects often play an important role, for instance, in recombination processes or high field transport. While a variety of techniques are available to assess the density and energy levels of impurities, other properties, such as the recombination mechanisms of the defects, escape observation. We report on the direct measurement of hot electrons generated by trap-assisted Auger-Meitner recombination (TAAR) in GaN p-i-n diodes. By performing electron emission spectroscopy (EES) on diodes with surfaces activated to negative electron affinity by cesium, we observe the expected overflow electrons of p-i-n diodes under low current injection. However, when operating the devices at higher current densities, as low as ∼25 A/c⁢m 2 , we measure the emission of high-energy electrons. At variance with the observed hot electrons in light-emitting diodes (LEDs) using EES, the hot electrons generated in p-i-n diodes at our tested currents cannot be from eeh Auger-Meitner recombination due to the diodes' significantly lower carrier densities compared to those in LEDs. During our measurements, we observe the emission of accumulated electrons with energies ∼0.42 eV, ∼0.99 eV, ∼1.43 eV, and ∼2.32 eV above the conduction-band minimum (CBM) at various bias conditions, suggesting the existence of conduction-band features in GaN at these energies where electrons can be long-lived, such as satellite-valley minima and inflection points. We also measure incompletely relaxed hot electrons approaching energies 1.97 ± 0.13 eV and 2.94 ± 0.13 eV above the CBM, as the diodes are biased to high currents, suggesting at least some of the TAAR partaking defects have an energy level ≳1.97 eV and ≳2.94 eV away from either the conduction or valence band edges. Additionally, at our highest operating currents, we measure hot electrons with energies 3.28 ± 0.13 eV above the CBM, providing direct evidence of TAAR processes involving shallow impurities. This unexpected observation of TAAR in GaN p-i-n diodes spotlights the importance of further studies of defects in GaN and the necessity to incorporate the multi-phonon emission, radiative, and TAAR capture steps of defect-assisted recombination cycles into device modeling. Furthermore, this experiment demonstrates the applicability of the simplest semiconductor structures, p-i-n diodes, as a test bed to study the rich recombination physics of semiconductor materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗