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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 289 records · Page 16
All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

Nanoscale ultrafast lattice modulation with a free-electron laser

Ultrafast optical laser-based techniques have enabled the probing of atomistic processes at their intrinsic temporal scales with femto- and attosecond resolution. However, the long wavelengths of optical lasers have prevented their interrogation and manipulation with nanoscale spatial specificity. Advances in hard X-ray free-electron lasers have enabled progress in developing X-ray transient-grating spectroscopy, a technique that aims to coherently control elementary excitations with nanoscale X-ray standing waves. Thus far, the realization of this technique at the nanoscale has been a challenge. Here we demonstrate X-ray transient-grating spectroscopy with spatial periods of the order of 10 nm via the subfemtosecond synchronization of two hard X-ray pump pulses at a precisely controlled crossing angle. This creates a thermal grating and preferentially excites coherent longitudinal acoustic phonon modes with the transient-grating wavevector. On probing with a third, variably delayed, X-ray pulse with the same photon energy, time-and-wavevector-resolved measurements of the modulation of the induced scattering intensity provide evidence of ballistic thermal transport at nanometre scales. Finally, these results highlight the potential of X-ray transient gratings as a powerful platform for studying nanoscale transport in condensed matter and the coherent control of nanoscale dynamics.

nonlinear optics↗
DOE OSTI2020

Bulk and Nanocrystalline Cesium Lead-Halide Perovskites as Seen by Halide Magnetic Resonance

Lead-halide perovskites increasingly mesmerize researchers because they exhibit a high degree of structural defects and dynamics yet nonetheless offer an outstanding (opto)electronic performance on par with the best examples of structurally stable and defect-free semiconductors. This highly unusual feature necessitates the adoption of an experimental and theoretical mindset and the reexamination of techniques that may be uniquely suited to understand these materials. Surprisingly, the suite of methods for the structural characterization of these materials does not commonly include nuclear magnetic resonance (NMR) spectroscopy. The present study showcases both the utility and versatility of halide NMR and NQR (nuclear quadrupole resonance) for probing the structure and structural dynamics of CsPbX 3 (X = Cl, Br, I), in both bulk and nanocrystalline forms. The strong quadrupole couplings, which originate from the interaction between the large quadrupole moments of, e.g., the 35 Cl, 79 Br, and 127 I nuclei, and the local electric-field gradients, are highly sensitive to subtle structural variations, both static and dynamic. The quadrupole interaction can resolve structural changes with accuracies commensurate with synchrotron X-ray diffraction and scattering. It is shown that space-averaged site-disorder is greatly enhanced in the nanocrystals compared to the bulk, while the dynamics of nuclear spin relaxation indicates enhanced structural dynamics in the nanocrystals. The findings from NMR and NQR were corroborated by ab initio molecular dynamics, which point to the role of the surface in causing the radial strain distribution and disorder. These findings showcase a great synergy between solid-state NMR or NQR and molecular dynamics simulations in shedding light on the structure of soft lead-halide semiconductors.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Dynamic structural views in solar energy materials by femtosecond electron diffraction

Solar materials convert light into other forms of energy through excited state processes occurring on ultrafast time and atomic length scales. Understanding and controlling such nonequilibrium processes is essential for applications ranging from photovoltaics to photocatalysis. These processes are commonly studied by transient optical techniques, which resolve charge carrier dynamics. However, optical spectroscopy does not directly probe the atomic-scale motions that play a central role in the ultimate functionality of these materials. Filling this missing gap, ultrafast electron and x-ray scattering techniques enable monitoring of structural dynamics in materials with femtosecond time resolution. In this work, we focus on the use of ultrafast electron diffraction (UED) techniques to probe photoinduced energy conversion dynamics in solar energy materials. First, we discuss the use of UED as an ultrafast lattice thermometer allowing a direct probe of nonradiative relaxations such as hot carrier cooling and Auger recombination. Second, we present a time-resolved atomic pair distribution function analysis enabled by UED, which uncovers lattice deformations arising from excitation localization in materials. Finally, we provide an outlook looking toward new approaches for resolving in situ energy conversion dynamics and uncovering structure–property relationships in solar energy materials.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Nanometer-Scale Acoustic Wave Packets Generated by Stochastic Core-Level Photoionization Events

We demonstrate that the absorption of femtosecond hard x-ray pulses excites quasispherical, high-amplitude, and high-wave-vector coherent acoustic phonon wave packets using an all hard-x-ray pump-probe scattering experiment. The time- and momentum-resolved diffuse scattering signal is consistent with an ensemble of 3D strain wave packets induced by the rapid electron cascade dynamics following photoionization at uncorrelated excitation centers. We quantify key parameters of this process, including the localization size of the stress field and the photon energy conversion efficiency into elastic energy. The parameters are determined by the photoelectron and Auger electron cascade dynamics, as well as the electron-phonon interaction. In particular, we obtain the localization size of the observed strain wave packet to be 1.5 and 2.5 nm for bulk SrTiO 3 and KTaO 3 single crystals, respectively. The results provide crucial information on the mechanism of x-ray energy deposition into matter and shed light on the shortest collective length scales accessible to coherent acoustic phonon generation using x-ray excitation. Published by the American Physical Society 2024

36 MATERIALS SCIENCE↗
DOE OSTI2026

Dynamic control of quantum phases in two-dimensional materials via Floquet engineering

The dynamical engineering of quantum states through periodic optical driving, known as Floquet engineering, has emerged as a powerful frontier in condensed matter physics, offering a pathway to realize material properties inaccessible in static equilibrium. This review provides a comprehensive overview of recent theoretical and experimental advances in the optical manipulation of two-dimensional (2D) quantum materials. We begin by systematically reviewing the evolution of the field from its pioneering applications in graphene and twisted moiré superlattices, highlighting the experimental realization of the light-induced anomalous Hall effect (AHE) to the complex spin-valley physics in transition metal dichalcogenides (TMDs). Furthermore, we briefly examine recent advances in 2D magnetic materials, demonstrating how optical driving can actively compete with intrinsic magnetism to dynamically switch magnetic orders and topological invariants. Moreover, we discuss the emerging frontiers of multi-frequency driving, quantum optimal control theory (QOCT), and ultrafast lightwave electronics. We highlight how tailored waveforms, such as bicircular light fields, and sub-cycle attosecond control can selectively break spatial symmetries to generate novel nonlinear photocurrents, mitigate dissipation, and extend the boundaries of quantum control well beyond the perturbative steady-state regime. Finally, we summarize the key experimental challenges for Floquet engineering, including effects such as heating and scattering, which limit coherent quantum control.

Wang, Wenpeng [Northeastern University, Shenyang, ↗
DOE OSTI2020

Liquid-phase mega-electron-volt ultrafast electron diffraction

The conversion of light into usable chemical and mechanical energy is pivotal to several biological and chemical processes, many of which occur in solution. To understand the structure–function relationships mediating these processes, a technique with high spatial and temporal resolutions is required. Here, we report on the design and commissioning of a liquid-phase mega-electron-volt (MeV) ultrafast electron diffraction instrument for the study of structural dynamics in solution. Limitations posed by the shallow penetration depth of electrons and the resulting information loss due to multiple scattering and the technical challenge of delivering liquids to vacuum were overcome through the use of MeV electrons and a gas-accelerated thin liquid sheet jet. To demonstrate the capabilities of this instrument, the structure of water and its network were resolved up to the 3rd hydration shell with a spatial resolution of 0.6 Å; preliminary time-resolved experiments demonstrated a temporal resolution of 200 fs.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2025

Plasmon Dynamics Driven by Aggregation of Tris(2,2′-bipyridine)ruthenium(II)-Functionalized Gold Nanoparticles Probed by XANES and Transient Absorption Spectroscopy

Energy conversion dynamics is critical for advancing next-generation photovoltaics, optoelectronics, and light-harvesting technologies. Noble metal plasmonic nanoparticles play a pivotal role as nanoscale electromagnetic confinement structures, driving photon-induced chemical reactions. In this study, we explore the effects of [Ru(bpy) 3 ] 2+ functionalization and aggregation on citrate-capped gold nanoparticles (AuNPs) of 40 and 100 nm diameters, focusing on molecule-plasmon interactions and their influence on electronic and energy dissipation properties. X-ray absorption near-edge spectroscopy (XANES) revealed that [Ru(bpy) 3 ] 2+ functionalization induces controlled aggregation without altering the oxidation state of gold. A more pronounced white-line intensity is observed in 40 nm AuNPs, consistent with greater s–p–d hybridization and a higher density of surface states, likely influenced by both nanoparticle size and aggregation. Transient absorption (TA) spectroscopy highlights faster electron–phonon relaxation dynamics in aggregated 40 nm nanoparticles, which is attributed to increased electron delocalization and more efficient coupling to the phonon bath. In contrast, 100 nm nanoparticles exhibit minimal changes due to a lower degree of aggregation. Interestingly, we observe that enhanced electron–phonon coupling in aggregated nanoparticles coincides with a slowing of electron–electron scattering. These observations suggest a competitive interplay between the two relaxation pathways, where enhanced energy transfer to the lattice in aggregated systems can suppress electronic thermalization. In conclusion, these findings underscore the critical role of nanoparticle size, aggregation, and molecule–surface interactions in modulating plasmonic dynamics and excited-state lifetimes and further provide valuable insights into designing tailored plasmonic systems with transformative potential for sensing, catalysis, and energy conversion.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Nonresonant Raman Control of Ferroelectric Polarization

Important advances is recently made in the search for materials with complex multi-phase landscapes that host photoinduced metastable collective states with exotic functionalities. In almost all cases so far, the desired phases are accessed by exploiting light–matter interactions via the imaginary part of the dielectric function through above-bandgap or resonant mode excitation. Nonresonant Raman excitation of coherent modes is experimentally observed and proposed for dynamic material control, but the resulting atomic excursion is limited to perturbative levels. Here, in this study, this challenge is overcome by employing nonresonant ultrashort pulses with low photon energies well below the bandgap. Using mid-infrared pulses, ferroelectric reversal is induced in lithium niobate, and the large-amplitude mode displacements are characterized through femtosecond stimulated Raman scattering and second harmonic generation. This approach, validated by first-principle calculations, defines a novel method for synthesizing hidden phases with unique functional properties and manipulating complex energy landscapes at reduced energy consumption and ultrafast speeds.

Shi, Jiaojian [Stanford Univ., CA (United States);↗
DOE OSTI2026

Room temperature sodium diffusion in sodium iron phosphate investigated with neutron scattering

Sodium iron phosphate, Na x FePO 4 , is currently one of the most promising cathode materials for sodium ion batteries. Here we employ a systematic approach using three neutron scattering techniques to investigate temperature dependent properties with a focus on the charge transfer processes. Two distinct Na + diffusive motions are observed with quasielastic neutron scattering, including room temperature motion. These processes correspond to rapid double jumps through extrinsic vacancy sites of ∼6 Å along with the more fundamental nearest neighbor jumps of 3.1 Å. Experimental observations of room temperature ionic diffusion are highly desirable, as the diffusion pathways are naturally well suited for efficient transport. Inelastic neutron scattering was used to probe the vibrational density of states that assist in the ionic and electronic (polaronic) transport processes, which are further supported with density functional theory. Neutron diffraction examines the disordering of the sodium sublattice upon transition to the solid-solution phase, which is believed to enhance the overall kinetics during sodium insertion/extraction. Finally, 57 Fe Mössbauer spectroscopy measurements probes polaron hopping and the local structural evolution that modifies the electron density surrounding the redox active iron sites. This study sheds light on the temperature induced atomic scale dynamics that occur in olivine Na x FePO 4 .

Novak, Eric [Swarthmore College, Swarthmore, PA (U↗
DOE OSTI2020

Holographic wavefront sensors

A brief historical review of the first designs of holographic wavefront sensors (WFS’s) and the concepts lying in their basis is presented. The main directions in the development of these sensors are highlighted and considered. One of these directions implies a two-stage transition from the use of several separate measuring channels with holograms filtering only one Zernike mode: first to the use of one channel with a multiplexed hologram filtering several first Zernike modes, and then to filtering the entire set of Zernike modes with the aid of one combined multiplexed hologram. Another line of research in this field (related to the first one) is the optimisation of the filter hologram structure in order to reduce cross-modulation interferences, increase multiplexing level, etc. One more line of research implements principles of dynamic holography by introducing spatial light modulators into the WFS composition. Hence, the advantages of time multiplexing of holograms can be used. The approach developed by G. Andersen’s team, aimed at adapting the holographic WFS design for operation as an element of adaptive optical system with a zonal corrector, as well as an approach implying development of hybrid holographic sensors, are considered separately. The results of the authors’ studies of holographic WFS’s with application of the methods of Fourier holography (i.e., holography of focused beams, in particular, using diffuse scatterers in a hologram recording channel) are also reported. (paper)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2021

Switching of the electron-phonon interaction in 1 T –VSe 2 assisted by hot carriers

We apply an intense infrared laser pulse in order to perturb the electronic and vibrational states in the three-dimensional charge density wave material 1T-VSe 2 . Ultrafast snapshots of the light-induced hot carrier dynamics and nonequilibrium quasiparticle spectral function are collected using time- and angle-resolved photoemission spectroscopy. Furthermore, the hot carrier temperature and time-dependent electronic self-energy are extracted from the time-dependent spectral function, revealing that incoherent electron-phonon interactions heat the lattice above the charge density wave critical temperature on a timescale of (200 ± 40) fs. Density functional perturbation theory calculations establish that the presence of hot carriers alters the overall phonon dispersion and quenches efficient low-energy acoustic phonon scattering channels, which results in a new quasiequilibrium state that is experimentally observed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

M-STAR: Magnetism second target advanced reflectometer at the Spallation Neutron Source

M-STAR is a next generation polarized neutron reflectometer with advanced capabilities. A new focusing guide concept is optimized for samples with dimensions down to a millimeter range. A proposed hybrid pulse-skipping chopper will enable experiments at constant geometry at one incident angle in a broad range of wavevector transfer Q up to 0.3 A –1 for specular, off-specular, and GISANS measurements. M-STAR will empower nanoscience and spintronics studies routinely on small samples (~2 × 2 mm 2 ) and of atomic-scale thickness using versatile experimental conditions of magnetic and/or electric fields, light, and temperature applied in situ to novel complex device-like nanosystems with multiple buried interfaces. M-STAR will enable improved grazing incidence diffraction measurements, as a surface-sensitive depth-resolved probe of, e.g., the out-of-plane component of atomic magnetic moments in ferromagnetic, antiferromagnetic, and more complex structures as well as in-plane atomic-scale structures inaccessible with contemporary diffractometry and reflectometry. New horizons will be opened by the development of an option to probe near-surface dynamics with inelastic grazing incidence scattering in the time-of-flight mode. These novel options in combination with ideally matched parameters of the second target station will place M-STAR in the world’s leading position for high resolution polarized reflectometry.

47 OTHER INSTRUMENTATION↗
DOE OSTI2024

Design of a Thomson scattering diagnostic for the SMall Aspect Ratio Tokamak (SMART)

Here, we describe the design of a Thomson scattering (TS) diagnostic to be used on the SMall Aspect Ratio Tokamak (SMART). SMART is a spherical tokamak being commissioned in Spain that aims to explore positive triangularity and negative triangularity plasma scenarios at a low aspect ratio. The SMART TS diagnostic is designed to operate at high spatial resolution, 6 mm scattering length in the low-field side and 9 mm in the high-field side regions, and a wide dynamic range, electron temperature from 1 eV to 1 keV and density from 5 x 10 18 m -3 to 1 x 10 20 m -3 ⁠, to resolve large gradients formed at the plasma edge and in the scrape-off layer (SOL) under different triangularities and low aspect ratios. A 2 J @1064 nm laser will be used that is capable of operating in the burst mode at 1, 2, and 4 kHz to investigate fast phenomena and at 30 Hz to study 1 s (or more) long discharges. The scattered light will be collected over an angular range of 60° – 120° from 28 spatial points in the midplane covering the entire plasma width and the outer midplane SOL. Each scattering signal will be spectrally resolved on five wavelength channels of a polychromator to obtain the electron temperature measurement. We will also present a method to monitor in situ laser alignment in the core during calibrations and plasma operations.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Nanostructural and rheological transitions of pH-responsive supramolecular systems involving a zwitterionic amphiphile and a triamine

Supramolecular aqueous complexes of a synthesized zwitterionic surfactant, 2-(dimethyl(octadecyl)ammonio)acetate (stearyl betaine) and diethylenetriamine, have been found to display pH-tunable rheological properties without the need for a co-surfactant. For this supramolecular system, the dynamically changing interplay among the constituents is responsible for the rich phase behavior including hollow nanotubules, bilayers, and vesicles. A further hypothesis is that hollow nanotubular structure is highly desirable for achieving chain entanglement geometries with reduced mesh size. The rheological properties of the suspension were measured using a rotational rheometer. An analysis using zero-shear viscosities at various temperatures as well as differential scanning calorimetry(DSC) helped shed light on thermodynamic and phase transitions taking place. The morphology of the suspension was analyzed by using a combination of small angle x-ray scattering(SAXS) and atomic force microscopy(AFM). Large steady-shear viscosities (up to ~160 Pa.s) and viscoelastic behavior was observed in acidic conditions which diminished upon increasing the pH. A novel analysis consisting of measured thermodynamic quantities such as activation energy(E a ) and enthalpy of transition(ΔH T ) further allude to the rich pH-sensitive nanoarchitecture of the system. Rather than commonly observed wormlike micelles, hollow nanotubules, as long as 1.6 µm were observed at pH 4 which disintegrated to bilayer sheets and vesicles upon increasing pH. Finally, gaining a comprehensive understanding from all the results, a transition mechanism between different suspension architectures was proposed.

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

Dynamic mode decomposition of nonequilibrium electron-phonon dynamics: accelerating the first-principles real-time Boltzmann equation

Abstract Nonequilibrium dynamics governed by electron–phonon ( e -ph) interactions plays a key role in electronic devices and spectroscopies and is central to understanding electronic excitations in materials. The real-time Boltzmann transport equation (rt-BTE) with collision processes computed from first principles can describe the coupled dynamics of electrons and atomic vibrations (phonons). Yet, a bottleneck of these simulations is the calculation of e –ph scattering integrals on dense momentum grids at each time step. Here we show a data-driven approach based on dynamic mode decomposition (DMD) that can accelerate the time propagation of the rt-BTE and identify dominant electronic processes. We apply this approach to two case studies, high-field charge transport and ultrafast excited electron relaxation. In both cases, simulating only a short time window of ~10% of the dynamics suffices to predict the dynamics from initial excitation to steady state using DMD extrapolation. Analysis of the momentum-space modes extracted from DMD sheds light on the microscopic mechanisms governing electron relaxation to a steady state or equilibrium. The combination of accuracy and efficiency makes our DMD-based method a valuable tool for investigating ultrafast dynamics in a wide range of materials.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Multiscale simulations of electron and ion dynamics in self-irradiated silicon

The interaction of energetic ions with the electronic and ionic system of target materials is an interesting but challenging multiscale problem, and understanding of the early stages after impact of heavy, initially charged ions is particularly poor. At the same time, energy deposition during these early stages determines later formation of damage cascades. In this work, we address the multiscale character by combining real-time time-dependent density functional theory for electron dynamics with molecular dynamics simulations of damage cascades. Our first-principles simulations prove that core electrons affect electronic stopping and have an unexpected influence on the charge state of the projectile. We show that this effect is absent for light projectiles, but dominates the stopping physics for heavy projectiles. By parametrizing an inelastic energy loss friction term in the molecular dynamics simulations using our first-principles results, we also show a qualitative influence of electronic stopping physics on radiation-damage cascades.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Probing the Short-Distance Structure of the Quark-Gluon Plasma with Energy Correlators

Energy-energy correlators (EECs) are promising observables to study the dynamics of jet evolution in the quark-gluon plasma (QGP) through its imprint on angular scales in the energy flux of final-state particles. We carry out the first complete calculation of EECs using realistic simulations of high-energy heavy-ion collisions and dissect the different dynamics underlying the final distribution through analyses of jet propagation in a uniform medium. The EECs of γ -jets in heavy-ion collisions are found to be enhanced by the medium response from elastic scatterings instead of induced gluon radiation at large angles. In the meantime, EECs are suppressed at small angles due to energy loss and transverse momentum broadening of jet shower partons. These modifications are further shown to be sensitive to the angular scale of the in-medium interaction, as characterized by the Debye screening mass. Experimental verification and measurement of such modifications will shed light on this scale and the short-distance structure of the QGP in heavy-ion collisions. Published by the American Physical Society 2024

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2023

Photometry of Outer Solar System Objects from the Dark Energy Survey. I. Photometric Methods, Light-curve Distributions, and Trans-Neptunian Binaries

We report the methods of and initial scientific inferences from the extraction of precision photometric information for the >800 trans-Neptunian objects (TNOs) discovered in the images of the Dark Energy Survey (DES). Scene-modeling photometry is used to obtain shot-noise-limited flux measures for each exposure of each TNO, with background sources subtracted. Comparison of double-source fits to the pixel data with single-source fits are used to identify and characterize two binary TNO systems. A Markov Chain Monte Carlo method samples the joint likelihood of the intrinsic colors of each source as well as the amplitude of its flux variation, given the time series of multiband flux measurements and their uncertainties. A catalog of these colors and light-curve amplitudes A is included with this publication. We show how to assign a likelihood to the distribution q(A) of light-curve amplitudes in any subpopulation. Using this method, we find decisive evidence (i.e., evidence ratio <0.01) that cold classical (CC) TNOs with absolute magnitude 6 < H$_{r}$ < 8.2 are more variable than the hot classical (HC) population of the same H$_{r}$, reinforcing theories that the former form in situ and the latter arise from a different physical population. Resonant and scattering TNOs in this H$_{r}$ range have variability consistent with either the HCs or CCs. DES TNOs with H$_{r}$ < 6 are seen to be decisively less variable than higher-H$_{r}$ members of any dynamical group, as expected. More surprising is that detached TNOs are decisively less variable than scattering TNOs, which requires them to have distinct source regions or some subsequent differential processing.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗