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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 397 records · Page 22
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Real-time interfacial electron dynamics revealed through temporal correlations in x-ray photoelectron spectroscopy

We present a novel technique to monitor dynamics in interfacial systems through temporal correlations in x-ray photoelectron spectroscopy (XPS) signals. To date, the vast majority of time-resolved x-ray spectroscopy techniques rely on pump–probe schemes, in which the sample is excited out of equilibrium by a pump pulse, and the subsequent dynamics are monitored by probe pulses arriving at a series of well-defined delays relative to the excitation. By definition, this approach is restricted to processes that can either directly or indirectly be initiated by light. It cannot access spontaneous dynamics or the microscopic fluctuations of ensembles in chemical or thermal equilibrium. Enabling this capability requires measurements to be performed in real (laboratory) time with high temporal resolution and, ultimately, without the need for a well-defined trigger event. The time-correlation XPS technique presented here is a first step toward this goal. The correlation-based technique is implemented by extending an existing optical-laser pump/multiple x-ray probe setup by the capability to record the kinetic energy and absolute time of arrival of every detected photoelectron. The method is benchmarked by monitoring energy-dependent, periodic signal modulations in a prototypical time-resolved XPS experiment on photoinduced surface-photovoltage dynamics in silicon, using both conventional pump–probe data acquisition, and the new technique based on laboratory time. The two measurements lead to the same result. The findings provide a critical milestone toward the overarching goal of studying equilibrium dynamics at surfaces and interfaces through time correlation-based XPS measurements.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2024

Toward ultrafast soft x-ray spectroscopy of organic photovoltaic devices

Novel ultrafast x-ray sources based on high harmonic generation and at x-ray free electron lasers are opening up new opportunities to resolve complex ultrafast processes in condensed phase systems with exceptional temporal resolution and atomic site specificity. In this perspective, we present techniques for resolving charge localization, transfer, and separation processes in organic semiconductors and organic photovoltaic devices with time-resolved soft x-ray spectroscopy. We review recent results in ultrafast soft x-ray spectroscopy of these systems and discuss routes to overcome the technical challenges in performing time-resolved x-ray experiments on photosensitive materials with poor thermal conductivity and low pump intensity thresholds for nonlinear effects.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2024

High energy electron diffraction instrument with tunable camera length

Ultrafast electron diffraction (UED) stands as a powerful technique for real-time observation of structural dynamics at the atomic level. In recent years, the use of MeV electrons from radio frequency guns has been widely adopted to take advantage of the relativistic suppression of the space charge effects that otherwise limit the temporal resolution of the technique. Nevertheless, there is not a clear choice for the optimal energy for a UED instrument. Scaling to beam energies higher than a few MeV does pose significant technical challenges, mainly related to the inherent increase in diffraction camera length associated with the smaller Bragg angles. In this study, we report a solution by using a compact post-sample magnetic optical system to magnify the diffraction pattern from a crystal Au sample illuminated by an 8.2 MeV electron beam. Our method employs, as one of the lenses of the optical system, a triplet of compact, high field gradients (>500 T/m), small-gap (3.5 mm) Halbach permanent magnet quadrupoles. Shifting the relative position of the quadrupoles, we demonstrate tuning the magnification by more than a factor of two, a 6× improvement in camera length, and reciprocal space resolution better than 0.1 Å –1 in agreement with beam transport simulations.

47 OTHER INSTRUMENTATION↗
DOE OSTI2025

Filling data analysis gaps in time-resolved crystallography by machine learning

There is a growing understanding of the structural dynamics of biological molecules fueled by x-ray crystallography experiments. Time-resolved serial femtosecond crystallography (TR-SFX) with x-ray Free Electron Lasers allows the measurement of ultrafast structural changes in proteins. Nevertheless, this technique comes with some limitations. One major challenge is the quality of data from TR-SFX measurements, which often faces issues like data sparsity, partial recording of Bragg reflections, timing errors, and pixel noise. To overcome these difficulties, conventionally, large volumes of data are collected and grouped into a few temporal bins. The data in each bin are then averaged and paired with the mean of their corresponding jittered timestamps. This procedure provides one structure per bin, resulting in a limited number of averaged structures for the entire time interval spanned by the experiment. Therefore, the information on ultrafast structural dynamics at high temporal resolution is lost. This has initiated research for advanced methods of analyzing experimental TR-SFX data beyond the standard binning and averaging method. To address this problem, we use a machine learning algorithm called Nonlinear Laplacian Spectral Analysis (NLSA), which has emerged as a promising technique for studying the dynamics of complex systems. In this work, we demonstrate the power of this algorithm using synthetic x-ray diffraction snapshots from a protein with significant data incompleteness, timing uncertainties, and noise. Our study confirms that NLSA is a suitable approach that effectively mitigates the effects of these artifacts in TR-SFX data and recovers accurate structural dynamics information hidden in such data.

Trujillo, Justin (ORCID:0000000285505360)↗
DOE OSTI2020

Ultrashort XUV pulse absorption spectroscopy of partially oxidized cobalt nanoparticles

High-order harmonic generation (HHG) based transient extreme ultraviolet (XUV) absorption spectroscopy is an emerging technique to trace photoinduced charge carrier dynamics in condensed phase materials with femtosecond and even attosecond temporal resolution and elemental specificity. However, its application to nanoparticulate samples that are relevant, for example, for novel photocatalytic light harvesting concepts, has been limited. This is in part due to the challenge to produce residual-free samples on ultrathin, XUV-transparent substrates as well as a widespread understanding that sparsely distributed nanoparticles do not provide sufficient contrast for XUV absorption measurements. Here, we present static XUV absorption spectra of partially oxidized Co nanowire-structures with diameters of approximately 4.5 nm and lengths between 10 and 40 nm, recorded with an ultrashort pulse HHG light source. Nanoparticles are synthesized by the agglomeration of Co atoms inside superfluid helium droplets, followed by surface deposition and oxidation in ambient air. The method is uniquely suited for residual-free synthesis of transition metal nanowires and their deposition on ultrathin substrates. Analysis by high-resolution transmission electron microscopy reveals the formation of CoO nanowires with regions of unoxidized Co in their interior. The nanoparticle samples are investigated in an HHG-driven ultrafast XUV absorption setup. Despite the low surface coverage of only 23%, the recorded spectrum exhibits a distinct absorption feature at the Co M 2,3 (2p) edge near 60 eV with a peak height of about 40 mOD. Finally, the results support the feasibility of table-top ultrafast transient XUV absorption studies of photoinduced dynamics in transition metal oxide nanoparticles with sub-monolayer surface coverage.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Robust analysis of space-, time-, and energy-resolved soft x-ray measurements of magnetically confined fusion plasmas (invited)

A novel compact multi-energy soft x-ray (ME-SXR) diagnostic based on the PILATUS3 100K x-ray detector has been developed in collaboration between the Princeton Plasma Physics Laboratory and the University of Wisconsin-Madison and tested on the Madison Symmetric Torus (MST) reversed-field pinch. This solid-state photon-counting detector consists of a two-dimensional array of ~100 000 pixels for which the lower photon absorption cutoff energy can be independently set, allowing it to be configured for a unique combination of simultaneous spatial, spectral, and temporal resolution of ~1 cm, 100 eV, and 500 Hz, respectively. The diagnostic is highly versatile and can be readily adapted to diverse plasma operating conditions and scientific needs without any required downtime. New results from improved-confinement and quasi-single helicity plasmas in the MST demonstrate how the detector can be applied to study multiple aspects of the evolution of magnetically confined fusion-grade plasmas. These include observing the evolution of thermal emissivity, characterizing the energy of mid-Z excitation lines, extracting the T e profile, and observing the evolution of non-thermal populations. A technique for integrating the ME-SXR diagnostic into an integrated data analysis framework based on Bayesian inference is also presented. As a result, this allows ME-SXR measurements to be combined with data for complementary diagnostics in order to simultaneously infer Te and nZ from all available information.

47 OTHER INSTRUMENTATION↗
DOE OSTI2021

Improved imaging using Mn He- α x rays at OMEGA EP

In this paper, we report on a crystal based x-ray imaging system fielded at the OMEGA EP laser facility. This new system has a pointing accuracy of +/100 μm, a temporal resolution down to 100 ps (depending on backlighter characteristics), variable magnification, and a spatial resolution of 21.9 µm at the object plane at a magnification of 15×. The system is designed to use a crystal along the crystal plane that satisfies the Bragg condition for the x ray of interest. The thin crystal is then bent into a spherical geometry and attached to a glass backing substrate to hold it in the diagnostic, and the x rays are imaged onto a charge coupled device. We report on data acquired with the new Los Alamos National Laboratory supplied spherical quartz crystal to image the Mn He-α 6.15 keV line emission.

Fiedler Kawaguchi, C. (ORCID:0000000175522370)↗
DOE OSTI2021

Mapping wave packet bifurcation at a conical intersection in CH 3 I by attosecond XUV transient absorption spectroscopy

Extreme ultraviolet (XUV) transient absorption spectroscopy has emerged as a sensitive tool for mapping the real-time structural and electronic evolution of molecules. Here, attosecond XUV transient absorption is used to track dynamics in the A-band of methyl iodide (CH 3 I). Gaseous CH 3 I molecules are excited to the A-band by a UV pump (277 nm, ~20 fs) and probed by attosecond XUV pulses targeting iodine I(4d) core-to-valence transitions. Owing to the excellent temporal resolution of the technique, passage through a conical intersection is mapped through spectral signatures of nonadiabatic wave packet bifurcation observed to occur at 15 ± 4 fs following UV photoexcitation. The observed XUV signatures and time dynamics are in agreement with previous simulations [H. Wang, M. Odelius, and D. Prendergast, J. Chem. Phys. 151, 124106 (2019)]. Furthermore, due to the short duration of the UV pump pulse, coherent vibrational motion in the CH 3 I ground state along the C-I stretch mode (538 ± 7 cm -1 ) launched by resonant impulsive stimulated Raman scattering and dynamics in multiphoton excited states of CH 3 I are also detected.

36 MATERIALS SCIENCE↗
DOE OSTI2021

First application of a digital mirror Langmuir probe for real-time plasma diagnosis

We report for the first time, a digital Mirror Langmuir Probe (MLP) has successfully sampled plasma temperature, ion saturation current, and floating potential together on a single probe tip in real time in a radio-frequency driven helicon linear plasma device. This is accomplished by feedback control of the bias sweep to ensure a good fit to I–V characteristics with a high frequency, high power digital amplifier, and field-programmable gate array controller. Measurements taken by the MLP were validated by a low speed I–V characteristic manually collected during static plasma conditions. Plasma fluctuations, induced by varying the axial magnetic field($\widetilde{f}$ = 10 Hz), were also successfully monitored with the MLP. Further refinement of the digital MLP pushes it toward a turn-key system that minimizes the time to deployment and lessens the learning curve, positioning the digital MLP as a capable diagnostic for the study of low radio-frequency plasma physics. These demonstrations bolster confidence in fielding such digital MLP diagnostics in magnetic confinement experiments with high spatial and adequate temporal resolution, such as edge plasma, scrape-off layer, and divertor probes.

47 OTHER INSTRUMENTATION↗
DOE OSTI2021

Two-dimensional retrieval methods for ultrafast imaging of molecular structure using laser-induced electron diffraction

Molecular structural retrieval based on electron diffraction has been proposed to determine the atomic positions of molecules with sub-angstrom spatial and femtosecond temporal resolutions. Given its success on small molecular systems, in this work, we point out that the accuracy of structure retrieval is constrained by the availability of a wide range of experimental data in the momentum space in all molecular systems. To mitigate the limitations, for laser-induced electron diffraction, here we retrieve molecular structures using two-dimensional (energy and angle) electron momentum spectra in the laboratory frame for a number of small molecular systems, which have previously been studied with 1D methods. Compared to the conventional single-energy or single-angle analysis, our 2D methods effectively expand the momentum range of the measured data. Besides utilization of the 2D data, two complementary methods are developed for consistency check on the retrieved results. Further, the 2D nature of our methods also offers a way of estimating the error from retrieval, which has never been explored before. Comparing with results from prior experiments, our findings show evidence that our 2D methods outperform the conventional 1D methods. Paving the way to the retrieval of large molecular systems, in which their tunneling ionization rates are challenging to obtain, we estimate the error of using the isotropic model in place of including the orientation-dependent ionization rate.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

Semi-empirical quantum optics for mid-infrared molecular nanophotonics

Nanoscale infrared (IR) resonators with sub-diffraction limited mode volumes and open geometries have emerged as new platforms for implementing cavity quantum electrodynamics at room temperature. The use of IR nanoantennas and tip nanoprobes to study strong light–matter coupling of molecular vibrations with the vacuum field can be exploited for IR quantum control with nanometer spatial and femtosecond temporal resolution. In order to advance the development of molecule-based quantum nanophotonics in the mid-IR, we propose a generally applicable semi-empirical methodology based on quantum optics to describe light–matter interaction in systems driven by mid-IR femtosecond laser pulses. The theory is shown to reproduce recent experiments on the acceleration of the vibrational relaxation rate in infrared nanostructures. It also provides physical insights on the implementation of coherent phase rotations of the near-field using broadband nanotips. We then apply the quantum framework to develop general tip-design rules for the experimental manipulation of vibrational strong coupling and Fano interference effects in open infrared resonators. We finally propose the possibility of transferring the natural anharmonicity of molecular vibrational levels to the resonator near-field in the weak coupling regime to implement intensity-dependent phase shifts of the coupled system response with strong pulses and develop a vibrational chirping model to understand the effect. The semi-empirical quantum theory is equivalent to first-principles techniques based on Maxwell’s equations, but its lower computational cost suggests its use as a rapid design tool for the development of strongly coupled infrared nanophotonic hardware for applications ranging from quantum control of materials to quantum information processing.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Spatiotemporal evolution of emission and absorption signatures in a laser-produced plasma

Here we report spatiotemporal evolution of emission and absorption signatures of Al species in a nanosecond (ns) laser-produced plasma (LPP). The plasmas were generated from an Inconel target, which contained ~0:4 wt. % Al, using 1064 nm, ≈6 ns full width half maximum pulses from an Nd:YAG laser at an Ar cover gas pressure of ≈34 Torr. The temporal distributions of the Al I (394.4 nm) transition were collected from various spatial points within the plasma employing time-of-flight (TOF) emission and laser absorption spectroscopy, and they provide kinetics of the excited state and ground state population of the selected transition. The emission and absorption signatures showed multiple peaks in their temporal profiles, although they appeared at different spatial locations and times after the plasma onset. The absorption temporal profiles showed an early time signature representing shock wave propagation into the ambient gas. We also used emission and absorption spectral features for measuring various physical properties of the plasma. The absorption spectral profiles are utilized for measuring linewidths, column density, and kinetic temperature, while emission spectra were used to measure excitation temperature. A comparison between excitation and kinetic temperature was made at various spatial points in the plasma. Our results highlight that the TOF measurements provide a resourceful tool for showing the spatiotemporal LPP dynamics with higher spatial and temporal resolution than is possible with spectral measurements but are difficult to interpret without additional information on excitation temperatures and linewidths. The combination of absorption and emission TOF and spectral measurements thus provides a more complete picture of LPP spatiotemporal dynamics than is possible using any one technique alone.

(140.3440) Laser-induced breakdown, (280.4788) Opt↗
DOE OSTI2022

Laser-driven, ion-scale magnetospheres in laboratory plasmas. I. Experimental platform and first results

We report magnetospheres are a ubiquitous feature of magnetized bodies embedded in a plasma flow. While large planetary magnetospheres have been studied for decades by spacecraft, ion-scale “mini” magnetospheres can provide a unique environment to study kinetic-scale, collisionless plasma physics in the laboratory to help validate models of larger systems. In this work, we present preliminary experiments of ion-scale magnetospheres performed on a unique high-repetition-rate platform developed for the Large Plasma Device at the University of California, Los Angeles. The experiments utilize a high-repetition-rate laser to drive a fast plasma flow into a pulsed dipole magnetic field embedded in a uniform magnetized background plasma. 2D maps of the magnetic field with high spatial and temporal resolution are measured with magnetic flux probes to examine the evolution of magnetosphere and current density structures for a range of dipole and upstream parameters. The results are further compared to 2D particle-in-cell simulations to identify key observational signatures of the kinetic-scale structures and dynamics of the laser-driven plasma. We find that distinct 2D kinetic-scale magnetopause and diamagnetic current structures are formed at higher dipole moments, and their locations are consistent with predictions based on pressure balances and energy conservation.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Design and construction of a compact, high-repetition-rate ultrafast electron diffraction instrument

We present the design and performance of a compact ultrafast electron diffraction instrument. The diffractometer provides a means of examining time-resolved ultrafast dynamical properties of solids. The system’s utilization is discussed in terms of instrument parameters and diffraction data from selected condensed matter samples. Here, the difractometer’s performance is highlighted in terms of detection sensitivity, instrumental temporal resolution, and the electron beam transverse coherence length. Following specific details of the construction, we present a practical discussion of parameters such as repetition rate and provide advice on general construction approaches for laboratory-based, keV ultrafast electron diffractometers. In addition, design guidance for constructing a compact electron gun source that is well-suited for studying diffraction from hard condensed matter is given. A unique data acquisition scheme, utilizing high laser repetition rates, is presented.

47 OTHER INSTRUMENTATION↗
DOE OSTI2022

Ultraefficient resistance switching between charge ordered phases in 1 T -TaS 2 with a single picosecond electrical pulse

Progress in high-performance computing demands significant advances in memory technology. Among novel memory technologies that promise efficient device operation on a sub-ns timescale, resistance switching between charge ordered phases of 1T-TaS 2 has shown to be potentially useful for development of high-speed, energy efficient nonvolatile memory devices. Measurement of the electrical operation of such devices in the picosecond regime is technically challenging and hitherto still largely unexplored. Here, we use an optoelectronic “laboratory-on-a-chip” experiment for measurement of ultrafast memory switching, enabling accurate measurement of electrical switching parameters with 100 fs temporal resolution. Photoexcitation and electro-optic sampling on a (Cd,Mn)Te substrate are used to generate and, subsequently, measure electrical pulse propagation with intra-band excitation and sub-gap probing, respectively. We demonstrate high contrast nonvolatile resistance switching from high to low resistance states of a 1T-TaS 2 device using single sub-2ps electrical pulses. Using detailed modeling, we find that the switching energy density per unit area is exceptionally small, E A =9.4 fJ/μm 2 . Finally, the speed and energy efficiency of an electronic “write” process place the 1T-TaS 2 devices into a category of their own among new generation nonvolatile memory devices.

42 ENGINEERING↗
DOE OSTI2022

Design of the high-yield time-gated x-ray hot-spot imager for OMEGA

Time-resolved x-ray self-emission imaging of hot spots in inertial confinement fusion experiments along several lines of sight provides critical information on the pressure and the transient morphology of the hot spot on the University of Rochester’s OMEGA Laser System. At least three quasi-orthogonal lines of sight are required to infer the tomographic information of the hot spots of deuterium–tritium cryogenic layered implosions. OMEGA currently has two time-gated x-ray hot-spot imagers: the time-resolved Kirkpatrick–Baez x-ray microscope and the single-line-of-sight, time-resolved x-ray imager (SLOS-TRXI). The time-gated x-ray hot-spot imager (XRHSI) is being developed for use on OMEGA as the third line of sight for the high-yield operation of up to 4 × 10 14 neutrons. XRHSI follows the SLOS-TRXI concept; however, it will have improved spatial and temporal resolutions of 5 μm and 20 ps, respectively. The simultaneous operation of the three instruments will provide 3-D reconstructions of the assembled hot-spot fuel at various times through peak thermonuclear output. The technical approach consists of a pinhole array imager and demagnifying time-dilation drift tube that are coupled to two side-by-side hybrid complementary metal–oxide semiconductor (hCMOS) image sensors. To minimize the background and to harden the diagnostics, an angled drift-tube assembly shifting the hCMOS sensors out of the direct line of sight and neutron shielding will be applied. As a result, the technical design space for the instrument will be discussed and the conceptual design will be presented.

47 OTHER INSTRUMENTATION↗
DOE OSTI2022

Fresnel zone plate point spread function approximation for zeroth order mitigation in millimetric field of view x-ray imaging

High spatial and temporal resolution x-ray radiography images are required at the National Ignition Facility (NIF) for high-energy density experiments. One technique that is in development to achieve the required resolution uses Fresnel zone plate (FZP) optics to image an object that is backlit by an x-ray source. The multiple FZP diffraction orders do not focus on the same plane, which increases the background and reduces the contrast. Understanding the point spread function of the different diffraction orders will allow the prediction of the expected background using simulations. We find that the two-dimensional point spread function of the FZP can be approximated by the addition of a sharp Gaussian with a disk. This allowed for the estimation of the background in NIF experimental images of Rayleigh–Taylor spikes and their interpretation. An alternative design of FZP is discussed to allow the inclusion of a zeroth order blocker to reduce the background.

Do, A. (ORCID:0000000174372147)↗
DOE OSTI2022

Design of an electron cyclotron emission diagnostics suite for COMPASS Upgrade tokamak

COMPASS Upgrade is a medium size and high field tokamak that is capable of addressing key challenges for reactor grade tokamaks, including power exhaust and advanced confinement scenarios. Electron cyclotron emission will be available among the first diagnostics to provide measurements of high spatial and temporal resolution of electron temperature profiles and electron temperature fluctuation profiles through a radial view. A separate oblique view at 12° from normal will be utilized to study non-thermal electrons. Both the radial and oblique views are envisioned to be located in a wide-angle midplane port, which has dimensions that enable simultaneous hosting of the front-end of their quasi-optical (QO) designs. Each QO design will have an in situ hot calibration source in the front-end to provide standalone and calibrated Te (R,t) measurements. The conceptual design for each QO system, the Gaussian beam analysis, and the details of the diagnostic channels are presented.

Instruments & Instrumentation↗