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DOE OSTI2024

Strong-Field Bloch Electron Interferometry for Band-Structure Retrieval

When Bloch electrons in a solid are exposed to a strong optical field, they are coherently driven in their respective bands where they acquire a quantum phase as the imprint of the band shape. If an electron approaches an avoided crossing formed by two bands, it may be split by undergoing a Landau-Zener transition. We here employ subsequent Landau-Zener transitions to realize strong-field Bloch electron interferometry (SFBEI), allowing us to reveal band structure information. In particular, we measure the Fermi velocity (band slope) of graphene in the vicinity of the K points as 1.07±0.04 nm fs –1 . As a result, we expect SFBEI for band structure retrieval to apply to a wide range of material systems and experimental conditions, making it suitable for studying transient changes in band structure with femtosecond temporal resolution at ambient conditions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2021

Watching a hydroperoxyalkyl radical (•QOOH) dissociate

A prototypical hydroperoxyalkyl radical (•QOOH) intermediate, transiently formed in the oxidation of volatile organic compounds, was directly observed through its infrared fingerprint and energy-dependent unimolecular decay to hydroxyl radical and cyclic ether products. Direct time-domain measurements of •QOOH unimolecular dissociation rates over a wide range of energies were found to be in accord with those predicted theoretically using state-of-the-art electronic structure characterizations of the transition state barrier region. Unimolecular decay was enhanced by substantial heavy-atom tunneling involving O-O elongation and C-C-O angle contraction along the reaction pathway. Master equation modeling yielded a fully a priori prediction of the pressure-dependent thermal unimolecular dissociation rates for the •QOOH intermediate—again increased by heavy-atom tunneling—which are required for global models of atmospheric and combustion chemistry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1989

Response of single junction GaAs/GaAs and GaAs/Ge solar cells to multiple doses of 1 MeV electrons

A comparison of the radiation tolerance of MOCVD-grown GaAs cells and GaAs/Ge cells was undertaken using 1 MeV electrons. The GaAs/Ge cells are somewhat more tolerant of 1 MeV electron irradiation and more responsive to annealing than are the GaAs/GaAs cells examined in this study. However, both types of cells suffer a greater degradation in efficiency than has been observed in other recent studies. The reason for this is not certain, but it may be associated with an emitter thickness which appears to be greater than desired. The deep level transient spectroscopy (DLTS) spectra following irradiation are not significantly different for the GaAs/Ge and the GaAs/GaAs cells, with each having just two peaks. The annealing behavior of these peaks is also similar in the two samples examined. It appears that no penalty in radiation tolerance, and perhaps some benefit, is associated with fabricating MOCVD GaAs cells on Ge substrates rather than GaAs substrates.

Meier, D. L.↗

NASA NTRS1994

Gamma-ray and millimeter-wave emissions from the 1991 June X-class solar flares

We have studied the spectacular 1991 June X-class flares using gamma-ray data from the Charged Particle Detectors (CPDs) of the Burst and Transient Source Experiment (BATSE) on the Compton Gamma Ray Observatory (CGRO) and 80 GHz millimeter data from Nobeyama, Japan. The CPDs were the only CGRO instrument that did not saturate during the extremely intense 1991 June 4 flare. We have shown that for this flare the CPDs respond to MeV photons, most of which are due to bremsstrahlung produced by relativistic electrons at the Sun. We have further shown that the gamma-ray and millimeter observations agree numerically if the 80 GHz radiation is gyrosynchrotron radiation produced by trapped electrons and the gamma rays are thick-target bremsstrahlung due to electrons precipitating out of the trap. The requirement that the trapping time obtained from the numerical comparison be consistent with the observed time profiles implies a magnetic field between about 200 and 300 G and an electron spectral index between about 3 to 5. By comparing the CPD observations with both the 80 GHz data and nuclear line data from the Energetic Gamma Ray Experiment Telescope (EGRET) and the Oriented Scintillation Spectroscopy Experiment (OSSE) on CGRO for the flares of June 4, 6, 9, and 11, we found that the ratio of the CPD counts to both the millimeter flux densities and the nuclear line fluences decreases with decreasing flare heliocentric angle. All of these flares were produced in the same active region. We interpreted this result in terms of a loop model in which the gyrosynchrotron emission is produced in the coronal portion of the loop where the electrons are kept isotropic by pitch angle scattering due to plasma turbulence, while the bremsstrahlung is produced by precipitating electrons that interact anisotropically. We found that the trapping time in the coronal portion is time dependent, reaching a minimum of about 10 s at the peak of the CPD count rate. We suggested the damping of the turbulence as a possible reason for the variation of the trapping time. turbulence as a possible reason for the variation of the trapping time.

Ramaty, Reuven↗

NASA NTRS2012

Multiscale Studies of the Three-Dimensional Dayside X-Line

We review recent experience from the Cluster, Double Star, and THEMIS missions for lessons that apply to the upcoming Magnetospheric Multiscale Mission (MMS) being developed for launch in 2014. On global scales, simulation and statistical studies lead to mean congurations of dayside reconnection, implying specific relative alignments of the inflow magnetic fields and X-line, with implications for MMS operations designed to maximize the number of close encounters with the diffusion region. At intermediate MHD-to-ion scales, reconstruction of features created by one or two X-lines have developed to the point where data from a cluster of spacecraft can determine their temporal trends and the approximate three-dimensional X-line structure. Recent petascale particle-in-cell (PIC) simulations of reconnection encompass three spatial dimensions with excellent resolution, and make striking predictions of electron scale physics that creates complex interacting flux ropes under component reconnection. High time resolution measurements from MMS will determine the detailed electron scale kinetics embedded within the global and MHDion scale contexts. These developments will lead to the refinement of our three-dimensional multiscale picture of reconnection, yielding improved understanding of the global, MHD, and local physics controlling the onset or quenching, variability, and mean rate of reconnection. This in turn will enable improved predictability of the structural features created by transient reconnection, and their space weather consequences.

Reconnection↗

DOE OSTI2022

A quantitative model of charge injection by ruthenium chromophores connecting femtosecond to continuous irradiance conditions

A kinetic framework for the ultrafast photophysics of tris(2,2-bipyridine)ruthenium(II) phosphonated and methyl-phosphonated derivatives is used as a basis for modeling charge injection by ruthenium dyes into a semiconductor substrate. By including the effects of light scattering, dye diffusion, and adsorption kinetics during sample preparation and the optical response of oxidized dyes, quantitative agreement with multiple transient absorption datasets is achieved on timescales spanning femtoseconds to nanoseconds. In particular, quantitative agreement with important spectroscopic handles—the decay of an excited state absorption signal component associated with charge injection in the UV region of the spectrum and the dynamical redshift of a ~500 nm isosbestic point—validates our kinetic model. Pseudo-first-order rate coefficients for charge injection are estimated in this work, with an order of magnitude ranging from 10 11 to 10 12 s –1 . The model makes the minimalist assumption that all excited states of a particular dye have the same charge injection coefficient, an assumption that would benefit from additional theoretical and experimental exploration. Here, we have adapted this kinetic model to predict charge injection under continuous solar irradiation and find that as many as 68 electron transfer events per dye per second take place, significantly more than prior estimates in the literature.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Ultrafast optical control of surface and bulk magnetism in magnetic topological insulator/antiferromagnet heterostructure

Abstract Optical control of the magnetic properties in topological insulator systems is an important step in applying these materials in ultrafast optoelectronic and spintronic schemes. In this work, we report the experimental observation of photo-induced magnetization dynamics in the magnetically doped topological insulator (MTI)/antiferromagnet (AFM) heterostructure composed of Cr-(Bi,Sb) 2 Te 3 /CrSb. Through proximity coupling to the AFM layer, the MTI displays a dramatically enhanced magnetism, with robust perpendicular magnetic anisotropy. When subjected to intense laser irradiation, both surface and bulk magnetism of the MTI are weakened by laser-induced heating of the lattice, however, at the surface, the deleterious heat effect is compensated by the strengthening of Dirac-hole-mediated exchange coupling as demonstrated by an unconventional pump-fluence-dependent exchange-bias effect. Through theoretical analyses, the sizes of exchange coupling energies are estimated in the MTI/AFM bilayer structure. The fundamentally different mechanisms supporting the surface and bulk magnetic order in MTIs allow a novel and distinctive photo-induced transient magnetic state with antiparallel spin configuration, which broadens the understanding of the magnetization dynamics of MTIs under ultrashort and intense optical excitation.

42 ENGINEERING↗

DOE OSTI2024

Directly Fused Porphyrin‐Tetracyanopentacenequinone Conjugates: Role of the Cross‐Conjugated, Powerful Electron Acceptor in Promoting Highly Efficient Charge Separation

Tetracyanopentacenequinone, a powerful electron acceptor, is fused directly to the porphyrin π-system to create a new class of donor-acceptor conjugates. Owing to the direct fusion and electron-deficient property of tetracyanopentacenequinone, strong intramolecular charge transfer both in the ground and excited states was witnessed. As a control, porphyrin fused with pentacenequinone was also investigated. Upon complete spectral and electrochemical characterization, the excited state properties were initially probed by time-dependent DFT studies, and the occurrence of electron transfer from different excited states was established. Free-energy calculations revealed higher exothermic electron transfer (>600 mV) than the control pentacenequinone-porphyrin systems. Pump-probe studies covering broad spatial and temporal regions revealed efficient excited state charge separation. This was unlike the control pentacenequinone-porphyrin system, where slow charge separation was witnessed only in the case of the zinc derivatives but not the free-base ones, followed by the populating of the triplet excited state. The lifetimes of the charge-separated states ranged between 30–500 ps depending on the solvent and metal ion in the porphyrin cavity. Nanosecond transient absorption studies established the charge recombination path to populate the triplet state of porphyrin or directly to the ground state as a function of solvent polarity and the nature of the conjugate. Furthermore, the significance of cross-conjugated tetracyanopentacenequinone fused directly to the porphyrin π system in promoting highly exothermic and efficient charge separation, irrespective of its cross conjugation, is borne out from this study.

Cross conjugation↗

NASA NTRS1991

Power electronics for low power arcjets

In anticipation of the needs of future light-weight low-power spacecraft, arcjet power electronics in the 100- to 400-W operating range were developed. Power topologies similar to those in the higher 2-kW and 5- to 30-kW power range were implemented, including a four-transistor bridge-switching circuit, current-mode pulse-width modulated control, and an output current averaging inductor with an integral pulse generation winding. Reduction of switching transients was accomplished using a low inductance power distribution network, and no passive snubber circuits were necessary for power switch protection. Phase shift control of the power bridge was accomplished using an improved pulse width modulation to phase shift converter circuit. These features, along with conservative magnetics designs, allowed power conversion efficiencies of greater than 92.5 percent to be achieved into resistive loads over the entire operating range of the converter.

Hamley, John A.↗

DOE OSTI2023

Elements of H-mode pedestal structure

Abstract This paper reviews current understanding of key physics elements that control the H-mode pedestal structure, which exists at the boundary of magnetically confined plasmas. The structure of interest is the width, height and gradient of temperature, density and pressure profiles in the pedestal. Emphasis is placed on understanding obtained from combined experimental, theoretical and simulation work and on results observed on multiple machines. Pedestal profiles are determined by the self-consistent interaction of sources, transport and magnetohydrodynamic limits. The heat source is primarily from heat deposited in the core and flowing to the pedestal. This source is computed from modeling of experimental data and is generally well understood. Neutrals at the periphery of the plasma provide the dominant particle source in current machines. This source has a complex spatial structure, is very difficult to measure and is poorly understood. For typical H-mode operation, the achievable pedestal pressure is limited by repetitive, transient magnetohydrodynamic instabilities. First principles models of peeling–ballooning modes are generally able to explain the observed limits. In some regimes, instability occurs below the predicted limits and these remain unexplained. Several mechanisms have been identified as plausible sources of heat transport. These include neoclassical processes for ion heat transport and several turbulent processes, driven by the steep pedestal gradients, as sources of electron and ion heat transport. Reduced models have successfully predicted the pedestal or density at the pedestal top. Firming up understanding of heat and particle transport remains a primary challenge for developing more complete predictive pedestal models.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2021

Mapping the catalytic conformations of an assembly-line polyketide synthase module

Assembly-line polyketide synthases, such as the 6-deoxyerythronolide B synthase (DEBS), are large enzyme factories prized for their ability to produce specific and complex polyketide products. By channeling protein-tethered substrates across multiple active sites in a defined linear sequence, these enzymes facilitate programmed small-molecule syntheses that could theoretically be harnessed to access countless polyketide product structures. Additionally, using cryogenic electron microscopy to study DEBS module 1, we present a structural model describing this substrate-channeling phenomenon. Our 3.2- to 4.3-angstrom-resolution structures of the intact module reveal key domain-domain interfaces and highlight an unexpected module asymmetry. We also present the structure of a product-bound module that shines light on a recently described “turnstile” mechanism for transient gating of active sites along the assembly line.

59 BASIC BIOLOGICAL SCIENCES↗

NASA NTRS1974

Amplitude steered array

A spin stabilized satellite has an electronically despun antenna array comprising a multiplicity of peripheral antenna elements. A high gain energy beam is established by connecting a suitable fraction or array of the elements in phase. The beam is steered or caused to scan by switching elements in sequence into one end of the array as elements at the other end of the array are switched out. The switching transients normally associated with such steering are avoided by an amplitude control system. Instead of abruptly switching from one element to the next, a fixed value of power is gradually transferred from the element at the trailing edge of the array to the element next to the leading edge.

Dietrich, F. J.↗

NASA NTRS1991

The performance of cable braids and terminations to lightning induced transients

The latest specification detailing the test waveforms for indirect lightning transients as applied to aircraft wiring systems specify very high voltages and currents. Although considerable data exists for measuring cable screen leakage using such methods as surface transfer impedance and bulk cable injection, there is little data on the likely core transient level that is likely to be induced from these threats. In particular, the new Waveform 5 at very high current levels (10 kA) is reputed to cause severe cable damage. A range of representative cables were made with various screen termination techniques and screening levels. These were tested first to determine their relative screening performance and then they were subjected to lightning transient testing to all the specified waveforms. Core voltages were measured for each test. Tests were also performed on bundles with fewer wires to determine the failure criteria with Waveform 5 and these tests also include flat conductor cables. The test showed that correctly terminated cable bundles performed well in all the tests and would provide a high level of protection to the electronic systems. The use of overbraides, provided the individual screens are well terminated, appears to be unnecessary.

Crofts, David↗

NASA NTRS2021

Mitigation of Finite Bandwidth Effects in Time-Division-Multiplexed SQUID Readout of TES Arrays

Time division multiplexing (TDM) is being developed as the readout technology of the X-ray integral field unit (X-IFU), a 3,168-pixel X-ray transition-edge sensor (TES) imaging spectrometer that is part of the European Space Agency's Athena satellite mission. Recent improvements in the low X-ray event count rate performance of TDM have been driven by increases in multiplexer bandwidth and the mitigation of settling transients. These methods and design changes have improved the 32-row multiplexed resolution of a NASA LPA 2.5a array from an initial (2.73 ± 0.03) eV to (1.97 ± 0.01) eV resolution at 5.9 keV. We discuss these recent advances in TDM readout, which have been implemented in an 8-column × 32-row spectrometer that will be deployed at the Lawrence Livermore National Laboratory electron beam ion trap (EBIT) facility, and present a model that will inform the design of future systems.

Transition-edge sensors↗

NASA NTRS1998

Particle Detectors and Data Analysis for Cusp Transient Features Campaign

On December 3, 1997, a rocket payload (36.152) was launched from Ny Alesund into the dark cusp at 0906:00 U (1206:00 LT) during an interval of southward B(sub Z), and positive B(sub y). Launch occurred during a time interval of northeastward moving auroral forms observed between 0845 and 0945 UT by ground-based meridian scanning photometers. Ground photometric measurements during the flight show that the payload passed over the poleward portion of the most intense 6300 A emissions of the dayside cusp/cleft region. Electrons of energy up to a few hundred eV were detected immediately upon instrument turn-on at an altitude of 205 km and throughout the flight until the payload reached an altitude of approximately 197 km on the downleg. Electron spectra were either quasithermal with peak energies approximately 100 eV or showed evidence of acceleration along the magnetic field line by potentials of 100-200 V. Precipitating ions were observed throughout much of the flight. Their spectra were broadly peaked in energy with the peak energy decreasing from approximately 500 eV to approximately 250 eV as the payload flew approximately westward over the dayside precipitationregion. Structure(spatial or temporal intensity variation) was observed between T + 180 s and T + approximately 400 s. At the rocket altitudes(less than 450km) the ions were observed to be precipitating. During the flight, the DMSPF-13 satellite passed through the all-sky imager field-of-view just poleward of the brightest dayside emissions enabling the identification of plasma sheet and boundary layer regions along the orbit. We thus conclude that particle fluxes detected by the rocket flight were either cusp plasma or boundary layer/mantle plasmajust poleward of the dayside cusp/cleft. Further investigation of the particle characteristics and their relationship to ionospheric convection patterns is continuing.

Sharber, James R.↗

DOE OSTI2021

Broadband 2DES detection of vibrational coherence in the S x state of canthaxanthin

The nonadiabatic mechanism that mediates nonradiative decay of the bright S 2 state to the dark S 1 state of carotenoids involves population of a bridging intermediate state, S x , in several examples. The nature of S x remains to be determined definitively, but it has been recently suggested that S x corresponds to conformationally distorted molecules evolving along out-of-plane coordinates of the isoprenoid backbone near a low barrier between planar and distorted conformations on the S 2 potential surface. Here, the electronic and vibrational dynamics accompanying the formation of S x in toluene solutions of the ketocarotenoid canthaxanthin (CAN) are characterized with broadband two-dimensional electronic spectroscopy (2DES) with 7.8 fs excitation pulses and detection of the linear polarization components of the third-order nonlinear optical signal. A stimulated-emission cross peak in the 2DES spectrum accompanies the formation of S x in <20 fs following excitation of the main absorption band. S x is prepared instantaneously, however, with excitation of hot-band transitions associated with distorted conformations of CAN’s isoprenoid backbone in the low frequency onset of the main absorption band. Vibrational coherence oscillation maps and modulated anisotropy transients show that S x undergoes displacements from the Franck–Condon S 2 state along out-of-plane coordinates as it passes to the S 1 state. The results are consistent with the conclusion that CAN’s carbonyl-substituted β-ionone rings impart an intramolecular charge-transfer character that frictionally slows the passage from S x to S 1 compared to carotenoids lacking carbonyl substitution. Despite the longer lifetime, the S 1 state of CAN is formed with retention of vibrational coherence after passing through a conical intersection seam with the S x state.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Demonstration of full-scale spatiotemporal diagnostics of solid-density plasmas driven by an ultra-short relativistic laser pulse using an X-ray free-electron laser

Understanding the complex plasma dynamics in ultra-intense relativistic laser–solid interactions is of fundamental importance for applications of laser–plasma-based particle accelerators, the creation of high-energy-density matter, understanding planetary science, and laser-driven fusion energy. However, experimental efforts in this regime have been limited by the lack of accessibility of over-critical densities and the poor spatiotemporal resolution of conventional diagnostics. Over the last decade, the advent of femtosecond brilliant hard X-ray free-electron lasers (XFELs) has opened new horizons to overcome these limitations. Here, for the first time, we present full-scale spatiotemporal measurements of solid-density plasma dynamics, including preplasma generation with tens of nanometer scale length driven by the leading edge of a relativistic laser pulse, ultrafast heating and ionization at the main pulse arrival, the laser-driven blast wave, and transient surface return current-induced compression dynamics up to hundreds of picoseconds after interaction. These observations are enabled by utilizing a novel combination of advanced X-ray diagnostics including small-angle X-ray scattering, resonant X-ray emission spectroscopy, and propagation-based X-ray phase-contrast imaging simultaneously at the European XFEL-HED beamline station.

Huang, Lingen [Helmholtz-Zentrum Dresden-Rossendor↗

DOE OSTI2021

The N-terminus of varicella-zoster virus glycoprotein B has a functional role in fusion

Varicella-zoster virus (VZV) is a medically important alphaherpesvirus that induces fusion of the virion envelope and the cell membrane during entry, and between cells to form polykaryocytes within infected tissues during pathogenesis. All members of the Herpesviridae , including VZV, have a conserved core fusion complex composed of glycoproteins, gB, gH and gL. The ectodomain of the primary fusogen, gB, has five domains, DI-V, of which DI contains the fusion loops needed for fusion function. We recently demonstrated that DIV is critical for fusion initiation, which was revealed by a 2.8Å structure of a VZV neutralizing mAb, 93k, bound to gB and mutagenesis of the gB-93k interface. To further assess the mechanism of mAb 93k neutralization, the binding site of a non-neutralizing mAb to gB, SG2, was compared to mAb 93k using single particle cryogenic electron microscopy (cryo-EM). The gB-SG2 interface partially overlapped with that of gB-93k but, unlike mAb 93k, mAb SG2 did not interact with the gB N-terminus, suggesting a potential role for the gB N-terminus in membrane fusion. The gB ectodomain structure in the absence of antibody was defined at near atomic resolution by single particle cryo-EM (3.9Å) of native, full-length gB purified from infected cells and by X-ray crystallography (2.4Å) of the transiently expressed ectodomain. Both structures revealed that the VZV gB N-terminus (aa72-114) was flexible based on the absence of visible structures in the cryo-EM or X-ray crystallography data but the presence of gB N-terminal peptides were confirmed by mass spectrometry. Notably, N-terminal residues 109 KSQD 112 were predicted to form a small α-helix and alanine substitution of these residues abolished cell-cell fusion in a virus-free assay. Importantly, transferring the 109 AAAA 112 mutation into the VZV genome significantly impaired viral propagation. These data establish a functional role for the gB N-terminus in membrane fusion broadly relevant to the Herpesviridae .

59 BASIC BIOLOGICAL SCIENCES↗