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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 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Resonant X-ray emission spectroscopy from broadband stochastic pulses at an X-ray free electron laser

Abstract Hard X-ray spectroscopy is an element specific probe of electronic state, but signals are weak and require intense light to study low concentration samples. Free electron laser facilities offer the highest intensity X-rays of any available light source. The light produced at such facilities is stochastic, with spikey, broadband spectra that change drastically from shot to shot. Here, using aqueous ferrocyanide, we show that the resonant X-ray emission (RXES) spectrum can be inferred by correlating for each shot the fluorescence intensity from the sample with spectra of the fluctuating, self-amplified spontaneous emission (SASE) source. We obtain resolved narrow and chemically rich information in core-to-valence transitions of the pre-edge region at the Fe K-edge. Our approach avoids monochromatization, provides higher photon flux to the sample, and allows non-resonant signals like elastic scattering to be simultaneously recorded. The spectra obtained match well with spectra measured using a monochromator. We also show that inaccurate measurements of the stochastic light spectra reduce the measurement efficiency of our approach.

Fuller, Franklin D. (ORCID:0000000237737087)↗
DOE OSTI2024

Resonant inelastic x-ray scattering in warm-dense Fe compounds beyond the SASE FEL resolution limit

Resonant inelastic x-ray scattering (RIXS) is a widely used spectroscopic technique, providing access to the electronic structure and dynamics of atoms, molecules, and solids. However, RIXS requires a narrow bandwidth x-ray probe to achieve high spectral resolution. The challenges in delivering an energetic monochromated beam from an x-ray free electron laser (XFEL) thus limit its use in few-shot experiments, including for the study of high energy density systems. Here we demonstrate that by correlating the measurements of the self-amplified spontaneous emission (SASE) spectrum of an XFEL with the RIXS signal, using a dynamic kernel deconvolution with a neural surrogate, we can achieve electronic structure resolutions substantially higher than those normally afforded by the bandwidth of the incoming x-ray beam. We further show how this technique allows us to discriminate between the valence structures of Fe and Fe2O3, and provides access to temperature measurements as well as M-shell binding energies estimates in warm-dense Fe compounds.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2023

Using electron energy-loss spectroscopy to measure nanoscale electronic and vibrational dynamics in a TEM

Electron energy-loss spectroscopy (EELS) can measure similar information to x-ray, UV–Vis, and IR spectroscopies but with atomic resolution and increased scattering cross-sections. Recent advances in electron monochromators have expanded EELS capabilities from chemical identification to the realms of synchrotron-level core-loss measurements and to low-loss, 10–100 meV excitations, such as phonons, excitons, and valence structures. EELS measurements are easily correlated with electron diffraction and atomic-scale real-space imaging in a transmission electron microscope (TEM) to provide detailed local pictures of quasiparticle and bonding states. This perspective provides an overview of existing high-resolution EELS (HR-EELS) capabilities while also motivating the powerful next step in the field—ultrafast EELS in a TEM. Ultrafast EELS aims to combine atomic-level, element-specific, and correlated temporal measurements to better understand spatially specific excited-state phenomena. Ultrafast EELS measurements also add to the abilities of steady-state HR-EELS by being able to image the electromagnetic field and use electrons to excite photon-forbidden and momentum-specific transitions. We discuss the technical challenges ultrafast HR-EELS currently faces, as well as how integration with in situ and cryo measurements could expand the technique to new systems of interest, especially molecular and biological samples.

Chemistry↗
DOE OSTI2025

Imaging nanoscale carrier, thermal, and structural dynamics with time-resolved and ultrafast electron energy-loss spectroscopy

Time-resolved and ultrafast electron energy-loss spectroscopy (EELS) is an emerging technique for measuring photoexcited carriers, lattice dynamics, and near-fields across femtosecond to microsecond timescales. When performed in either a specialized scanning transmission electron microscope or ultrafast electron microscope (UEM), time-resolved and ultrafast EELS can directly image charge carriers, lattice vibrations, and heat dissipation following photoexcitation or applied bias. Yet, recent advances in theoretical calculations and electron optics are often required to realize the full potential of ultrafast EEL spectrum imaging. Here, in this review, we present a comprehensive overview of the recent progress in the theory and instrumentation of time-resolved and ultrafast EELS. We begin with an introduction to the technique, followed by a physical description of the loss function. We outline approaches for calculating and interpreting ground-state and transient EEL spectra spanning low-loss plasmons to core-level excitations analogous to x-ray absorption. We then survey the current state of time-resolved and ultrafast EELS techniques beyond photon-induced near-field electron microscopy, highlighting abilities to image carrier and thermal dynamics. Finally, we examine future directions enabled by emerging technologies, including electron beam monochromation, in situ and operando cells, laser-free UEM, and high-speed direct electron detectors. These advances position time-resolved and ultrafast EELS as a critical tool for uncovering nanoscale dynamic processes in quantum materials and solar energy conversion devices.

Computational methods↗
DOE OSTI2026

Light-tight Skipper-CCDs for X-Ray Detection in Space

Skipper Charge-Coupled Devices (skipper-CCDs) are pixelated silicon detectors with deep sub-electron resolution. Their radiation hardness and capability to reconstruct energy deposits with unprecedented precision make them a promising technology for space-based X-ray astronomy. In this scenario, optical and near-infrared photons may saturate the sensor, distorting the reconstructed signal. We present a light-tight shield for skipper-CCDs to suppress optical backgrounds while preserving X-ray detection efficiency. We deposited thin aluminum layers on the CCD surface using an e-beam evaporator and evaluated their blinding performance across wavelengths from 650 to 1000 nm using a monochromator, as well as the X-ray transmission using an 55 Fe source. We find that 50 and 100 nm layers provide >99.6% light suppression, with no efficiency loss for 5.9 and 6.4 keV X-rays. In addition, we used Geant4 simulations to extend these results to a broader energy range and quantify the efficiency loss for different aluminum thicknesses. Results show that thin aluminum coatings are an effective, low-cost solution for optical suppression in skipper-CCDs intended for X-ray detection and space instrumentation.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2020

Light-responsive expression atlas reveals the effects of light quality and intensity in Kalanchoë fedtschenkoi, a plant with crassulacean acid metabolism

Abstract Background Crassulacean acid metabolism (CAM), a specialized mode of photosynthesis, enables plant adaptation to water-limited environments and improves photosynthetic efficiency via an inorganic carbon-concentrating mechanism. Kalanchoë fedtschenkoi is an obligate CAM model featuring a relatively small genome and easy stable transformation. However, the molecular responses to light quality and intensity in CAM plants remain understudied. Results Here we present a genome-wide expression atlas of K. fedtschenkoi plants grown under 12 h/12 h photoperiod with different light quality (blue, red, far-red, white light) and intensity (0, 150, 440, and 1,000 μmol m–2 s–1) based on RNA sequencing performed for mature leaf samples collected at dawn (2 h before the light period) and dusk (2 h before the dark period). An eFP web browser was created for easy access of the gene expression data. Based on the expression atlas, we constructed a light-responsive co-expression network to reveal the potential regulatory relationships in K. fedtschenkoi. Measurements of leaf titratable acidity, soluble sugar, and starch turnover provided metabolic indicators of the magnitude of CAM under the different light treatments and were used to provide biological context for the expression dataset. Furthermore, CAM-related subnetworks were highlighted to showcase genes relevant to CAM pathway, circadian clock, and stomatal movement. In comparison with white light, monochrome blue/red/far-red light treatments repressed the expression of several CAM-related genes at dusk, along with a major reduction in acid accumulation. Increasing light intensity from an intermediate level (440 μmol m-2 s-1) of white light to a high light treatment (1,000 μmol m–2 s–1) increased expression of several genes involved in dark CO2 fixation and malate transport at dawn, along with an increase in organic acid accumulation. Conclusions This study provides a useful genomics resource for investigating the molecular mechanism underlying the light regulation of physiology and metabolism in CAM plants. Our results support the hypothesis that both light intensity and light quality can modulate the CAM pathway through regulation of CAM-related genes in K. fedtschenkoi.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2023

Strongly Coupled Plasmon and Phonon Polaritons as Seen by Photon and Electron Probes

The ability to control and modify infrared excitations in condensed matter is of both fundamental and applied interest. Here we explore a system supporting low-energy excitations, in particular, mid-infrared localized plasmon modes and phonon polaritons that are tuned to be strongly coupled. We study the coupled modes by using far-field infrared spectroscopy, state-of-the-art monochromated electron energy-loss spectroscopy, numerical simulations, and analytical modeling. Here we demonstrate that the electron probe facilitates a precise characterization of polaritons constituting the coupled system, and enables an active control over the coupling and the resulting sample response both in frequency and space. Although far-field optical spectra can be substantially different from near-field electron energy-loss spectra, we show that a direct comparison is possible via postprocessing and right positioning of the electron beam. The resulting spectra allow us to evaluate the key parameters of the coupled system, such as the coupling strength, which we demonstrate to be probe independent. Our work establishes a rigorous description of the spectral features observed in light- and localized electron-based spectroscopies, which can be extended to the analysis of analogous optical systems with applications in heat management and electromagnetic field concentration or nanofocusing.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Infrared plasmonics: STEM-EELS characterization of Fabry-Pérot resonance damping in gold nanowires

Materials possessing strong midinfrared responses are of current interest because of their potential application to long-wavelength metamaterials, photonic devices, molecular detection, and catalysis. In this work, we utilize high-energy resolution (80 cm -1 , 10 meV) electron-energy-loss spectroscopy (EELS) in a monochromated and aberration-corrected scanning transmission electron microscope (STEM) to resolve multipolar surface plasmon resonances (SPRs), sometimes called Fabry-Pérot (FP) resonances, in gold nanowires with mode energies spanning from ~1000 to 8000 cm -1 . STEM-EELS provides access to these mid- to near-IR responses in a single acquisition, avoiding the difficulties inherent in obtaining the same data using near-field optical techniques. The experimentally measured FP resonance energies and linewidths, together with analytical modeling and full-wave numerical electrodynamics simulations, provide a comprehensive picture of the radiative and intrinsic contributions to the total damping rates. We find some FP modes with dephasing times >60fs, which is almost twice the longest previously reported plasmon dephasing time for individual Au nanoparticles in the infrared. The long dephasing times and the broad tunability of the FP resonance energies throughout the infrared region suggest additional opportunities for harnessing infrared plasmonic energy before dephasing occurs.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Infrared surface phonon nanospectroscopy of an interacting dielectric-particle–dielectric-substrate dimer using fast electrons

Refinements in energy monochromation and aberration correction in state-of-the-art scanning transmission electron microscopes has opened access to the far infrared regime for spectroscopic characterization at the nanoscale. At these low energies, the dielectric environment, such as a dielectric slab adjacent to the target specimen, may no longer play a passive role in the spectrum. Instead, the environment may itself host resonances that mix with those of the target and complicate interpretation of its spectral responses. This article explores a theoretical description of the coupling between the collective vibrational surface modes of a dielectric particle and dielectric slab of varying thickness for the purpose of elucidating the interacting phononic excitations in dielectric materials typical of inelastic electron scattering measurements in the infrared. Dynamical coordinates and a governing Hamiltonian are rigorously defined in the quasistatic limit to account for phonon mode mixing and forcing by an aloof electron probe, which travels along a grazing trajectory, parallel to the dielectric slab. As the spectral window of interrogation by fast electron probes has been extended down to thermal energies with unprecedented meV energy resolution, theoretical models like that presented herein are crucial for accurate interpretation of experimental data.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Enhanced Self-Seeding with Ultrashort Electron Beams

In this paper, we describe a new method to produce intensity stable, highly coherent, narrow-band x-ray pulses in self-seeded free electron (FEL) lasers. The approach uses an ultrashort electron beam to generate a single spike FEL pulse with a wide coherent bandwidth. The self-seeding monochromator then notches out a narrow spectral region of this pulse to be amplified by a long portion of electron beam to full saturation. In contrast to typical self-seeding where monochromatization of noisy self-amplified spontaneous emission pulses leads to either large intensity fluctuations or multiple frequencies, we show that this method produces a stable, coherent FEL output pulse with statistical properties similar to a fully coherent optical laser.

43 PARTICLE ACCELERATORS↗
DOE OSTI2021

Bent Laue crystal anatomy: new insights into focusing and energy-dispersion properties

X-ray Laue-type monochromators are common and essential optical components at many high-power X-ray facilities, e.g. synchrotron facilities. The X-ray optics of bent Laue crystals is a well developed area. An incident X-ray beam penetrating a bent Laue crystal will result in a diffracted beam with different angles and energies. There is a need for a way of organizing the rays that allows one to sort out the energy and spatial properties of the diffracted beam. The present work introduces a new approach for describing the general behaviour of bent Laue crystals from a ray-tracing point of view. This quasi-monochromatic beam approach provides an intuitive view of bent-crystal diffraction and leads to deeper understanding. It explains the energy and spatial properties of common and special cases of bent Laue optics, predicts phenomena that can improve energy-dispersion-related X-ray imaging techniques and provides a theoretical framework that makes ray-tracing simulation easier to realize.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Quantitative analysis of dislocations in 4H-SiC wafers using synchrotron X-ray topography with ultra-high angular resolution

Utilization of an Si(331) beam conditioner together with an Si(111) double-crystal monochromator (DCM) enables the angular resolution of synchrotron X-ray topography to be increased by an order of magnitude compared with grazing-incidence topography or back-reflection topography conducted with the DCM alone. This improved technique with extremely small beam divergence is referred to as synchrotron X-ray plane-wave topography (SXPWT). This study demonstrates that the rocking curve width of 4H-SiC 0008 in PWT is only 2.5" and thus the lattice distortion at the scale of 1" will significantly affect the diffracted intensity. This work reports the ultra-high angular resolution in SXPWT which enables detailed probing of the lattice distortion outside the dislocation core in 4H-SiC, where the sign of the Burgers vector can be readily determined through comparison with ray-tracing simulations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Compensation of heat load deformations using adaptive optics for the ALS upgrade: a wave optics study

In this paper, a realistic wave optics simulation method has been developed to study how wavefront distortions originating from heat load deformations can be corrected using adaptive X-ray optics. Several planned soft X-ray and tender X-ray insertion-device beamlines in the Advanced Light Source upgrade rely on a common design principle. A flat, first mirror intercepts the white beam; vertical focusing is provided by a variable-line-space monochromator; and horizontal focusing comes from a single, pre-figured, adaptive mirror. A variety of scenarios to cope with thermal distortion in the first mirror are studied by finite-element analysis. The degradation of the intensity distribution at the focal plane is analyzed and the adaptive optics that correct it is modeled. The range of correctable wavefront errors across the operating range of the beamlines is reported in terms of mirror curvature and spatial frequencies. The software developed is a one-dimensional wavefront propagation package made available in the OASYS suite, an adaptable, customizable and efficient beamline modeling platform.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2020

Combining Laue diffraction with Bragg coherent diffraction imaging at 34-ID-C

Measurement modalities in Bragg coherent diffraction imaging (BCDI) rely on finding a signal from a single nanoscale crystal object which satisfies the Bragg condition among a large number of arbitrarily oriented nanocrystals. However, even when the signal from a single Bragg reflection with ( hkl ) Miller indices is found, the crystallographic axes on the retrieved three-dimensional (3D) image of the crystal remain unknown, and thus localizing in reciprocal space other Bragg reflections becomes time-consuming or requires good knowledge of the orientation of the crystal. Here, the commissioning of a movable double-bounce Si (111) monochromator at the 34-ID-C endstation of the Advanced Photon Source is reported, which aims at delivering multi-reflection BCDI as a standard tool in a single beamline instrument. The new instrument enables, through rapid switching from monochromatic to broadband (pink) beam, the use of Laue diffraction to determine crystal orientation. With a proper orientation matrix determined for the lattice, one can measure coherent diffraction patterns near multiple Bragg peaks, thus providing sufficient information to image the full strain tensor in 3D. The design, concept of operation, the developed procedures for indexing Laue patterns, and automated measuring of Bragg coherent diffraction data from multiple reflections of the same nanocrystal are discussed.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2021

IRIXS Spectrograph: an ultra high-resolution spectrometer for tender RIXS

The IRIXS Spectrograph represents a new design of an ultra-high-resolution resonant inelastic X-ray scattering (RIXS) spectrometer that operates at the Ru L 3 -edge (2840 eV). First proposed in the field of hard X-rays by Shvyd'ko [(2015), Phys. Rev. A, 91, 053817], the X-ray spectrograph uses a combination of laterally graded multilayer mirrors and collimating/dispersing Ge(111) crystals optics in a novel spectral imaging approach to overcome the energy resolution limitation of a traditional Rowland-type spectrometer [Gretarsson et al. (2020), J. Synchrotron Rad. 27, 538–544]. In combination with a dispersionless nested four-bounce high-resolution monochromator design that utilizes Si(111) and Al 2 O 3 (110) crystals, an overall energy resolution better than 35 meV full width at half-maximum has been achieved at the Ru L 3 -edge, in excellent agreement with ray-tracing simulations.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2021

Diaboloidal mirrors: algebraic solution and surface shape approximations

A new type of optical element that can focus a cylindrical wave to a point focus (or vice versa) is analytically described. Such waves are, for example, produced in a beamline where light is collimated in one direction and then doubly focused by a single optic. A classical example in X-ray optics is the collimated two-crystal monochromator, with toroidal mirror refocusing. The element here replaces the toroid, and in such a system provides completely aberration free, point-to-point imaging of rays from the on-axis source point. We present an analytic solution for the mirror shape in its laboratory coordinate system with zero slope at the centre, and approximate solutions, based on bending an oblique circular cone and a bent right circular cylinder, that may facilitate fabrication and metrology.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2023

Mapping nanocrystal orientations via scanning Laue diffraction microscopy for multi-peak Bragg coherent diffraction imaging

The recent commissioning of a movable monochromator at the 34-ID-C endstation of the Advanced Photon Source has vastly simplified the collection of Bragg coherent diffraction imaging (BCDI) data from multiple Bragg peaks of sub-micrometre scale samples. Laue patterns arising from the scattering of a polychromatic beam by arbitrarily oriented nanocrystals permit their crystal orientations to be computed, which are then used for locating and collecting several non-co-linear Bragg reflections. The volumetric six-component strain tensor is then constructed by combining the projected displacement fields that are imaged using each of the measured reflections via iterative phase retrieval algorithms. Complications arise when the sample is heterogeneous in composition and/or when multiple grains of a given lattice structure are simultaneously illuminated by the polychromatic beam. Here, a workflow is established for orienting and mapping nanocrystals on a substrate of a different material using scanning Laue diffraction microscopy. The capabilities of the developed algorithms and procedures with both synthetic and experimental data are demonstrated. The robustness is verified by comparing experimental texture maps obtained with Laue diffraction microscopy at the beamline with maps obtained from electron back-scattering diffraction measurements on the same patch of gold nanocrystals. Such tools provide reliable indexing for both isolated and densely distributed nanocrystals, which are challenging to image in three dimensions with other techniques.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Toward a fully coherent tender and hard X-ray free-electron laser via cascaded EEHG in fourth-generation synchrotron light sources

Free-electron-laser-based beamlines utilize fully coherent laser pulses with extremely narrow bandwidth allowing direct use of X-rays without monochromators. This could be very beneficial for all users of current and future fourth-generation diffraction-limited synchrotron light sources (DL-SLSs) who need narrowband full-coherence high-brightness X-ray pulses. Based on our previous finding, i.e. that separating the two stages of echo-enabled harmonic generation (EEHG) with a few extra bending-magnet sections provides an effective way to increase the momentum compaction of chicane 1, one can simultaneously achieve adequate prebunching at extremely high harmonics as well as keep the energy modulation to the ideal minimum. This could open the door for cascaded EEHG, toward fully coherent tender and hard X-ray wavelengths. Built on our compact design of a twin-pulse seeding electron beam with an adjustable delay and timing jitter at the level of a few femtoseconds, a cascaded EEHG can be implemented, which includes two EEHG beamlines, where the radiation pulse generated by the first beamline with harmonic $h$ 1 could be used as the input seed laser pulse to the second beamline with harmonic $h$ 2 . Hence, the second radiator could potentially reach very high harmonics [$h$ = $h$ 1 (20)$h$ 2 (25–100)] from 500 to 2000, corresponding to tender and hard X-ray wavelengths. It is demonstrated that the cascaded EEHG scheme is compatible with almost any current or planned fourth-generation DL-SLS, with significant benefits for space-limited storage rings in particular. The main advantage is that this scheme requires almost no change of the storage-ring lattice and is fully compatible with other beamlines. Current proposals for rings with much longer straight sections would add self-amplified spontaneous emission as another viable option for storage-ring-based free-electron lasers.

36 MATERIALS SCIENCE↗