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Results for “Time-resolved light scattering spectroscopy”

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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9 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

Thomson Scattering with Gain

Thomson-scattering signals can be significantly modified by convective gains associated with the stimulated Raman scattering and stimulated Brillouin scattering instabilities as the scattered light traverses the probe beam. Gain results in amplification and narrowing of the red-shifted (i.e., Stokes) scattered light, whereas blue-shifted (anti-Stokes) features are depleted and broadened, making the relative prominence of these features a key signature of gain. Not accounting for instability growth has been a ubiquitous source of error in previous Thomson-scattering measurements.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2025

A Flat Analyzer Polycapillary Spectrometer for X-ray Absorption Spectroscopy of Dilute Transition Metals at X-ray-Free Electron Lasers

X-ray absorption spectroscopy (XAS) coupled with highly intense pulses from an X-ray-free electron laser (XFEL) can be used to track ultrafast chemical dynamics. Nonetheless, measurements for dilute samples (≤1 mM) have been exceptionally challenging, as scattering background signals dominate over the sample’s X-ray fluorescence. We show that femtosecond time-resolved XAS measurements of sub-millimolar transition metal solutions are now possible at the Linac Coherent Light Source (LCLS) using a high-throughput polycapillary XAS spectrometer, designed, developed, and commissioned at LCLS and the Stanford Synchrotron Radiation Lightsource (SSRL). The instrument integrates three polycapillary optics that collect and collimate X-ray fluorescence emitted from the interaction point with a high solid angle. X-ray collimated fluorescence is then selectively diffracted by coupled graphite analyzer crystals. As a result, the contribution of scattered photons is suppressed. Experiments at the Pt L 3 -edge on 0.1 mM aqueous K 2 PtCl 6 (delivered via a 100 μm liquid jet) were successfully performed in the laser pump X-ray probe configuration at the LCLS XCS and XPP instruments. We report the transient spectra of hexachloroplatinate within the first 10 ps after a 266 nm photoexcitation. We observed a short-lived reduced intermediate (≈2 ps). The polycapillary X-ray spectrometer at LCLS now enables the efficient study of the dynamics of ultradilute transition metals in solution. This capability opens the door to investigating plasmonic systems, photocatalysts, enzymes, and other scarce and dilute samples.

LCLS↗
DOE OSTI2026

The chemRIXS Instrument for Solution-Phase Resonant Inelastic X-ray Scattering at the Linac Coherent Light Source

The chemRIXS instrument at the Linac Coherent Light Source (LCLS) offers new opportunities for studying solution-phase systems with time-resolved soft X-ray spectroscopic methods such as resonant inelastic X-ray scattering (RIXS) using the recently commissioned high-repetition-rate LCLS-II X-ray free electron laser. The orders-of-magnitude X-ray flux improvement provided by the superconducting accelerator, combined with corresponding advances in the optical laser system and the liquid jet recirculation system, enables studies on dilute systems with high signal-to-noise compared to what was possible with the LCLS-I copper accelerator. These capabilities open up time-resolved X-ray absorption spectroscopy and RIXS to entirely new classes of samples, as well as enabling the development of new soft X-ray spectroscopic methods on liquid samples. An overview of the beamline components and the first LCLS-II commissioning results are presented.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Time-dependent phenomena in correlated materials

Understanding time-dependent processes and light-matter interaction in strongly correlated materials, and the interplay between electronic, orbital, vibrational, and spin degrees of freedom, is a cornerstone of condensed matter. These mechanisms can be proven by measuring the response of the systems to time-dependent perturbations. The corresponding time scales are dictated by the way light couples to the different excitations, and how these excitations exchange energy and momentum. Our research advances our understanding of these processes, and the interpretation of different equilibrium and time-resolved spectroscopies. Our project encompasses two main themes: (i) developing and refining computational techniques to study non-equilibrium spectroscopies including non-perturbative effects and (ii) applications to non-equilibrium phenomena. We have developed a new computational approach that works directly in the time domain: by including all the degrees of freedom involved in the scattering process (e.g. electrons, photons, neutrons), we solve the time dependent problem: a faithful numerical simulation of the experiment. By measuring the energy and momentum of the outgoing particles, we can extract information about the energy and momentum absorbed by the system. Prior to our work, people attempting to model and calculate non-equilibrium spectral functions relied on a description of the scattering cross section based on a formulation in the frequency domain, a treatment that is extremely cumbersome and complex. Our technique works in and out of equilibrium and can reproduce spectra by several spectroscopic techniques, such as time-resolved photoemission, neutron scattering, Raman, X-ray spectroscopies (RIXS, Auger, XAS, XMCD), and, by not relying on analytical approximations, yields results that reveal novel overlooked transient mechanisms. These tools provide sorely needed intuition for understanding the phenomenology of strongly correlated materials and will help experimentalists in identifying signatures of relevant excitations in pump-probe experiments, such as those conducted in DOE supported facilities.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Giant Electrostriction via Nanodomain Engineering in Relaxor Ferroelectric Polymers

Relaxor ferroelectric (RFE) polymers hold great promise for artificial muscles due to their high actuation strain, high loading stress, and fast response. However, the structural origin underlying their large electrostrictive deformation remains elusive. In this study, we investigate poly(vinylidene fluoride-co-trifluoroethylene) [P(VDF-TrFE)]-based RFE terpolymers, incorporating 1,1-chlorofluoroethylene (CFE) or chlorotrifluoroethylene (CTFE) (the terpolymers are denoted as terP-CFE and terP-CTFE, respectively) as termonomers. Although both terpolymers show similar semicrystalline morphology, drastically different electrostrictive properties are observed. Specifically, the terP-CFE annealed at 100 °C achieves a record-high transverse strain of ∼10.6%, whereas 100 °C-annealed terP-CTFE only shows a much lower actuation strain of ∼4.2% at the same poling field of 190 MV/m. To elucidate the origin of this difference, time-resolved wide-angle X-ray diffraction, small-angle X-ray scattering, and Fourier transform infrared experiments are performed during in situ electric poling. An RFE-to-ferroelectric (FE) crystal phase transition is observed for terP-CFE but is absent for terP-CTFE. Beyond the contribution of the crystalline phase, the oriented amorphous fraction and crystalline defects (e.g., taut-tie molecules) also play significant roles in enhancing electrostriction. In conclusion, this mechanistic insight provides a valuable foundation for the rational design of next-generation RFE polymers with tunable properties through defect engineering of their semicrystalline structures.

36 MATERIALS SCIENCE↗
DOE OSTI2025

X-ray Absorption Spectroscopy of Dilute Metalloenzymes at X-ray Free-Electron Lasers in a Shot-by-Shot Mode

X-ray absorption spectroscopy (XAS) of 3d transition metals provides important electronic structure information for many fields. However, X-ray-induced radiation damage under physiological temperature has prevented using this method to study dilute aqueous systems, such as metalloenzymes, as the catalytic reaction proceeds. Here we present a new approach to enable operando XAS of dilute biological samples and demonstrate its feasibility with K-edge XAS spectra from the Mn cluster in photosystem II and the Fe–S centers in photosystem I. This approach combines highly efficient sample delivery strategies and a robust signal normalization method with high-transmission Bragg diffraction-based spectrometers at X-ray free-electron lasers (XFELs) in a damage-free, shot-by-shot mode. These photon-out spectrometers have been optimized for discriminating the metal Mn/Fe Kα fluorescence signals from the overwhelming scattering background present on currently available detectors for XFELs that lack suitable energy discrimination. We quantify the enhanced performance metrics of the spectrometer and discuss its potential applications for acquiring time-resolved XAS spectra of biological samples during their reactions at XFELs.

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

Capturing Coupled Structural and Electronic Motions During Excited-State Intramolecular Proton Transfer via Computational Multiedge Resonant Inelastic X-ray Scattering

Proton-transfer processes build the foundation of many chemical processes. In Excited State Intramolecular Proton Transfer (ESIPT) processes the proton transfer process is impulsively started through light. Here, in this study, we explore the changes in coupled atomic and electronic motions during and following ESIPT through computational time-resolved Resonant Inelastic X-ray Scattering (trRIXS). Excited-state Ab Initio Molecular Dynamics (AIMD) simulations combined with Time-Dependent Density Functional Theory (TDDFT) calculations were performed for 10-hydroxybenzo[h]quinoline to obtain trRIXS signatures. RIXS at both the nitrogen and oxygen K-edges were computed to resolve the dynamics electronic structure from both the proton donor and acceptor perspective. The results show how RIXS can reveal the local electronic structure, the coupling between different electronic states and how electronic structure and coupling change during the proton transfer process. Additionally, we observe a strong correlation between spectral changes and structural changes during ESIPT.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Field-resolved observation of exciton coherence in a van der Waals magnet

The emergence of coherence among electronic quasiparticles underlies collective quantum phenomena from superconductivity to superradiance. In semiconductors, exciton coherence is generally thought to decay rapidly due to scattering and dephasing, limiting its persistence on ultrafast timescales. Here, in this work, we demonstrate a light-field-driven mechanism that creates and stabilizes exciton coherence in the layered antiferromagnet CrSBr. We directly record the coherent optical field emitted by excitons and track in real time how a deterministic phase, imprinted by the excitation laser, drives incoherent excitons to synchronize into a collective state. This ensemble remains phase coherent for more than 2 ps, whereas its resonance energy undergoes an ultrafast modulation mediated by spin and lattice interactions. The time-resolved field evolution indicates that the multiple peaks seen in conventional spectra originate from a single excitonic resonance subject to dynamic energy modulation. Our findings establish optical phase imprinting as a mechanism to control and sustain collective order in semiconducting magnets, bridging light-driven dynamics with excitonic and magnetic correlations in layered quantum materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Dynamics of the transition from the metastable tetragonal st12 to the diamond-cubic phase in germanium characterized by neutron spectroscopy

The complex phase diagram of germanium allows for exotic crystalline phases recoverable from high pressure. Among these, the tetragonal st12 phase is unusual as it shares characteristics with amorphous Ge resulting in desirable band-gap characteristics. Here, we leverage a high neutron flux and large volume pressure capabilities to characterize st12-Ge and its dynamics upon conversion to diamond-cubic Ge with inelastic neutron scattering. Here, we exploit the characteristics of time-of-flight neutron scattering for time-resolved investigations. This analysis may suggest the existence of a transient disordered state upon annealing befitting the known structural relationship between st12-Ge and amorphous Ge, a relationship that can open the potential for band-gap tuning.

Elemental semiconductors↗