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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 253 records · Page 14
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Spectroscopic investigation of early light emission from anode-initiated surface flashover in vacuum

Time-resolved optical emission spectroscopy is used to explore the early development of anode-initiated flashover in vacuum. An experimental apparatus for collecting flashover self-luminosity is introduced, which enables spatially resolved light collection from regions adjacent to the anode and cathode triple junctions. The emitted light is spectrally and temporally resolved utilizing an imaging spectrograph and a fast electronic shutter camera. The first light detectable from flashovers across both Rexolite and polytetrafluoroethylene (PTFE) insulators begins less than 10 ns prior to the flashover gap's impedance collapse and consists of faint broadband feature in primarily visible wavelengths. This suggests luminosity due to excitation in the solid, possibly occurring as a result of field emitted electrons. In the few nanoseconds leading up to and including the impedance collapse, the broadband spectrum grows in intensity and extends into the UV, eventually accompanied by a few emission lines of the insulator material. This is strong evidence that the early stages of anode-initiated flashover include surface layer breakdown of the insulator, as a contrast from cathode-initiated flashover, which is predominately an above-surface process. Spectra accumulated over longer exposures of PTFE flashovers indicate that, in the first few hundred nanoseconds after the impedance collapse, ions from the insulator material constitute the majority of the emission lines. Later, neutral and ionic metal species from the electrode contribute with similar prominence as well as molecular bands from diatomic carbon. Finally, a comparison is provided of the results of these studies to other spectroscopic investigations of vacuum flashover from the literature.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2024

Evaluation of silicon and indium gallium arsenide photodiodes as direct timing detectors for pulsed x-ray systems

Benchtop pulsed x-ray systems are commonly used to record dynamic material data on the order of nanoseconds, but pulse timing is often difficult to accurately determine. This study demonstrates that commercially available photodiodes can be used effectively for direct x-ray pulse detection without the need for visible light scintillators. X-ray pulses from four commercially available flash x-ray systems were quantified using one silicon and two indium gallium arsenide (InGaAs) photodiodes. The measured InGaAs pulse durations were strongly dependent on radiation dose in the non-linear operating regime, so the photodiodes were shielded to operate below the 2.5 V non-linear regime threshold. The average pulse duration and pulse arrival time jitter of the photodiodes for each x-ray source were within several nanoseconds with the exception of two sets of measurements that were affected by low instrument sensitivity and electrical noise. These results show that InGaAs photodiodes can be used as effective and repeatable stand-alone timing diagnostics for x-ray pulses as short as 20 ns or less.

47 OTHER INSTRUMENTATION↗
DOE OSTI2026

Rotational coherence dominates early-time dynamics and produces long-time revivals in the S 2 state of azulene

Here, the ultrafast dynamics of azulene have been debated for decades, with reported picosecond decay constants variously attributed to intramolecular vibrational redistribution (IVR), internal conversion, or rotational dephasing. Using polarization- and femtosecond time-resolved resonance-enhanced multiphoton ionization spectroscopy with a nanosecond delay window, we disentangle this long-standing inconsistency and show that the early 2–5 ps decay component arises entirely from the rotational dephasing of an excited-state wavepacket. Identical time constants extracted from the decay of the parallel signal and the rise of the perpendicular signal across multiple vibronic origins provide an unambiguous rotational anisotropy signature, eliminating the need for IVR-based interpretations. Extending the measurement window to 1.3 ns reveals well-structured J-type and C-type rotational coherence revivals in S 2 azulene on top of the well-documented fluorescence decay, demonstrating that both the short- and long-time dynamics contain information about the coherent rotational dynamics. These results show that azulene, and by extension polycyclic aromatic hydrocarbons, can sustain structured rotational coherence deep into the nanosecond regime, positioning PAHs as model systems for quantum-coherent wavepacket dynamics and providing a framework for probing coherence, decoherence, and rotational control in electronically rich molecular systems.

Zhan, Jie [University of Georgia, Athens, GA (Unit↗
DOE OSTI2020

Generation of gamma radiation by a subterawatt ultrashort laser pulse: optimisation of preplasma and pulse duration

We report an experimental and numerical study of the acceleration of electrons in a plasma interacting with a subterawatt laser pulse (intensity of ∼3 × 10{sup 18} W cm{sup −2} at a pulse duration of 50 fs). A preplasma layer on the surface of a molybdenum target is formed by an additional laser pulse with a duration of 8 ns and an intensity of ∼2 × 10{sup 12} W cm{sup −2}. It is shown that an increase in the laser pulse duration to 1700 fs at a constant energy (and a proportional decrease in intensity) leads to an increase in the yield of bremsstrahlung γ-radiation by more than an order of magnitude when the nanosecond pulse is ahead of the femtosecond one by 15 − 25 ns. Interferometry data and results of diagnostics of optical and γ-radiation of a plasma demonstrate that the collisional ionisation of atoms by electrons oscillating in the field of such a laser pulse plays an essential role in the formation of electron density profile. The sensitivity of the described effect to the level of amplified spontaneous emission is determined, despite the nanosecond pulse impact. Numerical simulations show that at a large pulse duration, the acceleration of electrons is stipulated by the beaking of plasma waves excited during stimulated Raman scattering of laser radiation. (paper)

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Temporal and spatial resolution of distal protein motions that activate hydrogen tunneling in soybean lipoxygenase

The enzyme soybean lipoxygenase (SLO) provides a prototype for deep tunneling mechanisms in hydrogen transfer catalysis. This work combines room temperature X-ray studies with extended hydrogen–deuterium exchange experiments to define a catalytically-linked, radiating cone of aliphatic side chains that connects an active site iron center of SLO to the protein–solvent interface. Employing eight variants of SLO that have been appended with a fluorescent probe at the identified surface loop, nanosecond fluorescence Stokes shifts have been measured. We report a remarkable identity of the energies of activation ( E a ) for the Stokes shifts decay rates and the millisecond C–H bond cleavage step that is restricted to side chain mutants within an identified thermal network. These findings implicate a direct coupling of distal protein motions surrounding the exposed fluorescent probe to active site motions controlling catalysis. While the role of dynamics in enzyme function has been predominantly attributed to a distributed protein conformational landscape, the presented data implicate a thermally initiated, cooperative protein reorganization that occurs on a timescale faster than nanosecond and represents the enthalpic barrier to the reaction of SLO.

Science & Technology - Other Topics↗
DOE OSTI2021

Filamentary surface plasma discharge flow length and time scales

Nanosecond surface dielectric barrier discharges (ns-SDBDs) are a class of plasma actuators that utilize a high-voltage pulse of nanosecond duration between two surface-mounted electrodes to create an electrical breakdown of air, along with rapid heating. These actuators usually produce multiple filaments when operated at high pulse frequencies, and the rapid heating leads to the formation of shock waves and complex flow fields. In this work we replicate a single filament of the ns-SDBDs and characterize the induced flow using velocity measurements from particle image velocimetry and density measurements from background-oriented schlieren. The discharge is produced by a high voltage electrical pulse between two copper electrodes on an acrylic base. A hot gas kernel characterizes the flow field formed close to the electrodes that expands and cools over time and a vortex ring that propagates away from the surface while entraining cold ambient fluid. The gas density deficit inside the kernel displays a power-law decay over time. Based on the observations, we develop a simplified theoretical model based on vortex-driven cooling and perform a scaling analysis to obtain the induced flow length and time scales. The results show that the cooling process's time scales correspond to a circulation-based time scale of the vortex ring, and the length scale of the kernel corresponds to the vortex ring radius. Furthermore, these findings can guide the choice of optimal filament spacing and pulse frequencies in the design, deployment, and operation of ns-SDBDs for flow control.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Examination of OH and H 2 O 2 production by uniform and non-uniform modes of dielectric barrier discharge in He/air mixture

In this work we have carried out a parametrical study of hydroxyl radical (OH) generation in nanosecond dielectric barrier discharge (DBD) in He/air mixture using a laser-induced fluorescence approach. Specifically, the foci of the study are the investigation of differences between uniform and non-uniform modes of the discharges and the difference in production of OH and H 2 O 2 Nanosecond-time scale imaging of the discharge shows transition from streamer to diffuse mode when applied electric field to the discharge gap approaches ~90 kV cm –1 . The results show that both OH production in the gas phase and downstream H 2 O 2 delivery rates to liquid depend on the discharge mode operation and are respectively 30% and 3 times higher for the non-uniform DBD compared to the diffuse discharge.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Beryllium-driven structural evolution at the divertor surface

Erosion of the beryllium first wall material in tokamak reactors has been shown to result in transport and deposition on the tungsten divertor. Experimental studies of beryllium implantation in tungsten indicate that mixed W–Be intermetallic deposits can form, which have lower melting temperatures than tungsten and can trap tritium at higher rates. To better understand the formation and growth rate of these intermetallics, we performed cumulative molecular dynamics (MD) simulations of both high and low energy beryllium deposition in tungsten. In both cases, a W–Be mixed material layer (MML) emerged at the surface within several nanoseconds, either through energetic implantation or a thermally-activated exchange mechanism, respectively. While some ordering of the material into intermetallics occurred, fully ordered structures did not emerge from the deposition simulations. Targeted MD simulations of the MML to further study the rate of Be diffusion and intermetallic growth rates indicate that for both cases, the gradual re-structuring of the material into an ordered intermetallic layer is beyond accessible MD time scales(≤1 μs). However, the rapid formation of the MML within nanoseconds indicates that beryllium deposition can influence other plasma species interactions at the surface and begin to alter the tungsten material properties. Therefore, beryllium deposition on the divertor surface, even in small amounts, is likely to cause significant changes in plasma-surface interactions and will need to be considered in future studies.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Ultra-fast transverse beam orbit control in LCLS copper linac. Part I

We report current and future experiments at LCLS require x-ray pulse trains of variable time separation on the nanosecond scale. For instance, the cavity-based XFEL (CBXFEL) will use up to 4 pulses separated by 218.5 ns, the X-ray Laser Oscillator (XLO) will use 15 to 25 ns spaced pulses, and the Matter under Extreme Conditions (MEC) experiments use pulse trains separated by 5 nanoseconds or less. In this paper, we demonstrate an ultra-fast e-beam trajectory control method based on transverse electro-magnetic (TEM) striplines and state-of-the-art power sources, to enhance LCLS operations in these regimes.

47 OTHER INSTRUMENTATION↗
DOE OSTI2021

Ab initio ultrafast spin dynamics in solids

Spin relaxation and decoherence is at the heart of spintronics and spin-based quantum information science. Currently, theoretical approaches that can accurately predict spin relaxation of general solids including necessary scattering pathways and are capable of nanosecond to millisecond simulation time are urgently needed. We present a first-principles real-time density-matrix approach based on Lindblad dynamics to simulate ultrafast spin dynamics for general solid-state systems. Through the complete first-principles descriptions of pump, probe, and scattering processes including electron-phonon, electron-impurity, and electron-electron scatterings with self-consistent electronic spin-orbit couplings, our method can directly simulate the ultrafast pump-probe measurements for coupled spin and electron dynamics over nanoseconds at any temperatures and doping levels. We first apply this method to a prototypical system GaAs and obtain excellent agreement with experiments. We found that the relative contributions of different scattering mechanisms and phonon modes differ considerably between spin and carrier relaxation processes. In sharp contrast to previous work based on model Hamiltonians, we point out that the electron-electron scattering is negligible at room temperature but becomes dominant at low temperatures for spin relaxation in n-type GaAs. We further examine ultrafast dynamics in novel spin-valleytronic materials: monolayer and bilayer WSe 2 with realistic defects. We find that spin relaxation is highly sensitive to local symmetry and chemical bonds around defects. For the bilayer WSe 2 , we identify the scattering pathways in ultrafast dynamics and determine relevant dynamical properties, essential to its utilization of unique spin-valley-layer locking effects. In conclusion, our work provides a predictive computational platform for spin dynamics in solids, which has potential for designing new materials ideal for spintronics and quantum information technology.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Structural study of hcp and liquid iron under shock compression up to 275 GPa

Here we combine nanosecond laser shock compression with in situ picosecond x-ray diffraction to provide structural data on iron up to 275 GPa. We constrain the extent of hcp-liquid coexistence, the onset of total melt, and the structure within the liquid phase. Our results indicate that iron, under shock compression, melts completely by 258(8) GPa. A coordination number analysis indicates that iron is a simple liquid at these pressure-temperature conditions. We also perform texture analysis between the ambient body-centered-cubic (bcc) α, and the hexagonal-closed-packed (hcp) high-pressure ε-phase. We rule out the Rong-Dunlop orientation relationship (OR) between the α and ε - phase s. However, we cannot distinguish between three other closely related ORs: Burger's, Mao-Bassett-Takahashi, and Potter's OR. The solid-liquid coexistence region is constrained from a melt onset pressure of 225(3) GPa from previously published sound speed measurements and full melt [246.5(1.8)–258(8) GPa] from x-ray diffraction measurements, with an associated maximum latent heat of melting of 623 J/g. This value is lower than recently reported theoretical estimates and suggests that the contribution to the earth's geodynamo energy budget from heat release due to freezing of the inner core is smaller than previously thought. Melt pressures for these nanosecond shock experiments are consistent with gas gun shock experiments that last for microseconds, indicating that the melt transition occurs rapidly.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Isomers and hindrances in No254: A touchstone for theories of superheavy nuclei

We report on a new spectroscopic study of the decay of high-K isomers in No152102254, a touchstone nucleus for testing models to understand the structure of superheavy nuclei. The experiment, performed using the Argonne gas-filled analyzer (AGFA), was geared toward resolving long-standing ambiguities in spin-parity and configuration assignments for the two- and four-quasiparticle (qp) intrinsic excitations identified in this nucleus. The isomer decay schemes are firmly established with the help of the highest-statistics γ-γ coincidence data collected to date, providing anchor points for competing theories. A newly measured half-life in the nanosecond range establishes a second 2-qp isomer in No254. The preferred decay pathways for the 2- and 4-qp isomers are discussed, providing new insights into the underlying hindrance mechanisms at play in these heavy nuclei. With firm configuration assignments, the intrinsic excitations in this deformed mass region provide stringent constraints and challenge the different theoretical approaches at play in understanding the structure of superheavy nuclei.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2021

Time Refraction of Spin Waves

Here, we present an experimental study of time refraction of spin waves (SWs) propagating in microscopic waveguides under the influence of time-varying magnetic fields. Using space- and time-resolved Brillouin light scattering microscopy, we demonstrate that the broken translational symmetry along the time coordinate results in a loss of energy conservation for SWs and thus allows for a broadband and controllable shift of the SW frequency. With an integrated design of SW waveguide and microscopic current line for the generation of strong, nanosecond-long, magnetic field pulses, a conversion efficiency up to 39% of the carrier SW frequency is achieved, significantly larger compared to photonic systems. Given the strength of the magnetic field pulses and its strong impact on the SW dispersion relation, the effect of time refraction can be quantified on a length scale comparable to the SW wavelength. Furthermore, we utilize time refraction to excite SW bursts with pulse durations in the nanosecond range and a frequency shift depending on the pulse polarity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Analytical and numerical studies of dark current in radiofrequency structures for short-pulse high-gradient acceleration

High-gradient acceleration is a key research area that could enable compact linear accelerators for future colliders, light sources, and other applications. In the pursuit of high-gradient operation, rf breakdown limits the attainable accelerating gradient in normal-conducting rf structures. Recent experiments at the Argonne Wakefield Accelerator suggest a promising approach: using short rf pulses with durations of a few nanoseconds. Experimental studies show that these 𝒪⁡(1⁢ ⁢ns) rf pulses can mitigate breakdown limitations, resulting in higher gradients. For example, an electric field of nearly 400 MV/m was achieved in an 𝑋-band photoemission gun driven by 6-ns-long rf pulses, with rapid rf conditioning and low dark current observed. Despite these promising results, the short-pulse regime remains an underexplored parameter space, and rf breakdown physics under nanosecond-long pulses requires further investigation. In this paper, we present analytical and numerical simulations of dark current dynamics in accelerating cavities operating in the short-pulse regime. We study breakdown-associated processes spanning different time scales, including field emission, multipacting, and plasma formation, using simulations of the 𝑋-band photogun cavities. The results reveal the advantages of using short rf pulses to reduce dark current and mitigate rf breakdown, offering a path toward a new class of compact accelerators with enhanced performance and reduced susceptibility to breakdown.

Linear accelerators↗
DOE OSTI2021

Visualization of shocked material instabilities using a fast-framing camera and XFEL four-pulse train

Many questions regarding dynamic materials could be answered by using time-resolved ultra-fast imaging techniques to characterize the physical and chemical behavior of materials in extreme conditions and their evolution on the nanosecond scale. In this work, we perform multi-frame phase-contrast imaging (PCI) of micro-voids in low density polymers under laser-driven shock compression. At the Matter in Extreme Conditions (MEC) Instrument at the Linac Coherent Light Source (LCLS), we used a train of four x-ray free electron laser (XFEL) pulses to probe the evolution of the samples. To visualize the void and shock wave interaction, here, we deployed the Icarus V2 detector to record up to four XFEL pulses, separated by 1-3 nanoseconds. In this work, we image elastic waves interacting with the micro-voids at a pressure of several GPa. Monitoring how the material’s heterogeneities, like micro-voids, dictate its response to a compressive wave is important for benchmarking the performances of inertial confinement fusion energy materials. For the first time in a single sample, we have combined an ultrafast x-ray framing camera and four XFEL pulse train to create an ultrafast movie of micro-void evolution under laser-driven shock compression. Eventually, we hope this technique will resolve the material density as it evolves dynamically under laser shock compression.

fusion↗
DOE OSTI2020

Reversible structural transformations in supercooled liquid water from 135 to 245 K

Water has many anomalous properties compared to “simple” liquids, and these anomalies are typically enhanced in supercooled water.1-3 While numerous models have been proposed, including the liquid-liquid critical point,4,5 the singularity-free scenario,6 and the stability limit conjecture,1 a molecular-level understanding remains elusive. The main difficulty in determining which, if any, of these models is correct is the limited amount of data in the relevant temperature and pressure ranges. For water at ambient pressures, which is the focus of this work, data is largely missing from 160 – 232 K (“No Man’s Land”) due to rapid crystallization.2,3 Whether rapid crystallization is just an experimental obstacle, or a fundamental problem signaling the inability of water to thermally equilibrate prior to crystallization is also a major unanswered question.5,7 Here, we investigate the structural transformations of transiently-heated, supercooled water with nanosecond time resolution using infrared vibrational spectroscopy. The experiments demonstrate three key results. First, water’s structure relaxes from its initial configuration to a “steady-state” configuration prior to the onset of crystallization over a wide temperature range. Second, water’s steady-state structure can be reproduced by a linear combination of two, temperature-independent structures that correspond to a “high-temperature liquid” and a “low-temperature liquid.” Third, the observed structural changes are reversible over the full temperature range. Taken together, these results show that supercooled water can equilibrate prior to crystallization for temperatures from the homogeneous nucleation temperature, TH ~232 K,3 down to the glass transition temperature (Tg ~ 136 K). Second, the results provide support for the hypothesis that supercooled water can be described as a mixture of two, structurally-distinct, interconvertible liquids from 135 K to 245 K.5,8-18

Kringle, Loni M.↗
DOE OSTI2022

Optical and photophysical properties of platinum benzoporphyrins with C 2v and D 2h symmetry

Platinum(II) mono- and di-benzoporphyrins carrying either ester or imide peripheral groups have been successfully synthesized. These benzoporphyrins possessing C 2v and D 2h symmetry were investigated using a range of techniques including UV-Vis and phosphorescence spectroscopy, differential pulse voltammetry, and transient absorption spectroscopy covering wide spatial and temporal ranges. Up to three oxidation and three reductions within the accessible potential window of dichlorobenzene were observed. Facile reductions for both mono- and dibenzoporphyrin derivatives, more so with imide peripheral substituents were witnessed. Computational studies were supportive of push-pull type interactions within these molecular systems. Here, the formation of triplet excited states within 5 ps after laser excitation was confirmed by femtosecond transient absorption studies. Nanosecond transient absorption studies coupled with phosphorescence lifetime studies revealed relatively rapid relaxation of the triplet excited states as compared to a controlled platinum porphyrin suggesting push-pull type interactions on a slower time scale.

DFT calculations↗
DOE OSTI2022

Free Energy Dependencies for Interfacial Electron Transfer from Tin-Doped Indium Oxide (ITO) to Molecular Photoredox Catalysts

John B. Goodenough proposed that interfacial electron transfer kinetics from main group metal oxides should be fundamentally different from that of transition metal oxides, an expectation that has not been widely tested. Herein, the kinetics for interfacial electron transfer from mesoporous transparent conductive oxide Tin-doped Indium Oxide (ITO) to four photoredox catalysts (PCs) were characterized in acetonitrile electrolytes. The photocatalysts had the form: [Ru(4,4ʹ-R 2 -2,2′-bipyridine) 2 (4,4ʹ-(PO 3 H 2 ) 2 -2,2′-bipyridine)] 2+ , where R was H, methoxy, tert -butyl, and Br. The impact of the surface binding group was characterized with [Ru(2,2′-bipyridine) 2 (4,4ʹ-(CO 2 H) 2 -bpy)] 2+ . The interfacial electron transfer reaction ITO(e − )∣PC + → ITO∣PC was quantified by nanosecond absorption spectroscopy as a function of the applied potential (and hence ‒Δ G °). Specific conditions of applied potential were identified where the kinetics were sensitive to the incident irradiance. A layer-by-layer method was used to insert ionic methylene bridge(s) between the PC and the oxide surface. Marcus-Gerischer analysis of the kinetic data indicates non-adiabatic interfacial electron transfer with total reorganization energies that increase when bridges were placed between the photocatalyst and the ITO surface.

Bangle, Rachel E.↗