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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 379 records · Page 21
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Tunable Plasma Linearizer for Compensation of Nonlinear Energy Chirp

The removal of undesired nonlinear time-energy correlation (energy chirp) present in relativistic electron beams is crucial for many accelerator-based scientific applications, such as free-electron lasers, high-energy electron radiography, and MeV ultrafast electron microscopy. Here, we propose and demonstrate that a low-density plasma section can be used as a passive “linearizer” to significantly compensate for the nonlinear energy chirp imprinted on a beam by the curvature of the radio-frequency field in a conventional accelerator. Physically, the passage of the beam through the plasma excites a strong quasi-cosinoidal longitudinal decelerating wakefield that acts to mitigate the beam’s nonlinear energy chirp by superimposing a reverse chirp on the beam. Time-resolved phase-space measurements, combined with high-fidelity three-dimensional particle-in-cell simulations show that the longitudinal phase space of the beam core is almost completely linearized, leading to a fourfold reduction of the beam overall energy spread from 0.148% to 0.036% (FWHM).

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2022

X-ray FEL linear accelerator design via start-to-end global optimization

An X-ray Free Electron Laser (FEL) prefers using an electron beam with low emittance, small energy spread, and a high core current to generate coherent radiation through an undulator. In order to attain such a high brightness beam, the linear accelerator beam dynamics design generally involves separate photoinjector optimization and linac optimization. In this paper, we propose a new beam dynamics design strategy based on global optimization with fast start-to-end simulations from the photocathode to the end of the accelerator. The new start-to-end model significantly reduces the simulation time and makes the global optimization practical. The global optimization method avoids the need to choose a single solution based on bunch length at the injector exit for the linac optimization and helps find the solution with unfavorable bunch length at the injector exit but better phase space distribution that can result in better final electron beam phase space distribution at the entrance of the undulator. Here, using the start-to-end global optimization, we showed in an application example, with a 100 pC beam that good transverse emittance and over kilo-Ampere final core current can be attained using a photoinjector that consists of a VHF gun and boosting RF cavities.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2026

New perspectives on materials and device dynamics using time-resolved full-field diffraction X-ray imaging

Understanding how materials evolve during synthesis, processing, or device operation requires experimental access to structural dynamics across wide ranges of length and time scales, often in bulk samples or even within packaged devices. Time-resolved full-field diffraction X-ray microscopy has recently emerged as a powerful way to meet this need by combining the penetration and structural sensitivity of X-ray diffraction with objective-lens-based magnification, sensitive high-resolution X-ray imaging detectors, and pump-probe and real-time imaging strategies. Advances in full-field X-ray diffraction microscopy, often termed dark-field X-ray microscopy (DFXM), enable simultaneous imaging of extended fields of view while retaining crystallographic selectivity. Time-resolved DFXM promises to enable advances in materials processing and dynamics, electrochemical and photochemical processes, and the design of electronic devices. This Perspective summarizes the key instrumental concepts that define the performance of these methods, including the choice of imaging optics, detector considerations, and the impact of source time structure at synchrotron light sources and X-ray free-electron lasers (XFELs). We discuss the simultaneous use of complementary imaging modes that are increasingly used in practice. The early demonstrations of the potential of time-resolved DFXM include real-time defect and grain-boundary dynamics during metal annealing, stroboscopic imaging of functional devices with high strain sensitivity, and ultrafast pump-probe implementations at XFELs that directly visualize acoustic-wave propagation and energy dissipation in bulk crystals.

Dark-field X-ray microscopy↗
DOE OSTI2023

A MHz X-ray diffraction set-up for dynamic compression experiments in the diamond anvil cell

An experimental platform for dynamic diamond anvil cell (dDAC) research has been developed at the High Energy Density (HED) Instrument at the European X-ray Free Electron Laser (European XFEL). Advantage was taken of the high repetition rate of the European XFEL (up to 4.5 MHz) to collect pulse-resolved MHz X-ray diffraction data from samples as they are dynamically compressed at intermediate strain rates (≤10 3 s −1 ), where up to 352 diffraction images can be collected from a single pulse train. The set-up employs piezo-driven dDACs capable of compressing samples in ≥340 µs, compatible with the maximum length of the pulse train (550 µs). Results from rapid compression experiments on a wide range of sample systems with different X-ray scattering powers are presented. A maximum compression rate of 87 TPa s −1 was observed during the fast compression of Au, while a strain rate of ∼1100 s −1 was achieved during the rapid compression of N 2 at 23 TPa s −1 .

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2022

Physically and chemically smooth cesium-antimonide photocathodes on single crystal strontium titanate substrates

The performance of x-ray free electron lasers and ultrafast electron diffraction experiments is largely dependent on the brightness of electron sources from photoinjectors. Here, the maximum brightness from photoinjectors at a particular accelerating gradient is limited by the mean transverse energy (MTE) of electrons emitted from photocathodes. For high quantum efficiency (QE) cathodes like alkali-antimonide thin films, which are essential to mitigate the effects of non-linear photoemission on MTE, the smallest possible MTE and, hence, the highest possible brightness are limited by the nanoscale surface roughness and chemical inhomogeneity. In this work, we show that high QE Cs 3 Sb films grown on lattice-matched strontium titanate (STO) substrates have a factor of 4 smoother, chemically uniform surfaces compared to those traditionally grown on disordered Si surfaces. We perform simulations to calculate roughness induced MTE based on measured topographical and surface-potential variations on the Cs 3 Sb films grown on STO and show that these variations are small enough to have no consequential impact on the MTE and, hence, the brightness.

43 PARTICLE ACCELERATORS↗
DOE OSTI2021

Measurements of nonequilibrium interatomic forces using time-domain x-ray scattering

Here, we demonstrate an experimental approach to determining the excited-state interatomic forces using femtosecond x-ray pulses from an x-ray free-electron laser. We determine experimentally the excited-state interatomic forces that connect photoexcited carriers to the nonequilibrium lattice dynamics in the prototypical Peierls-distorted material, bismuth. The forces are obtained by a constrained least-squares fit of a pairwise interatomic force model to the excited-state phonon dispersion relation as measured by the time- and momentum-resolved x-ray diffuse scattering. We find that photoexcited carriers weaken predominantly the nearest-neighbor forces, which drives the measured softening of the transverse acoustic modes throughout the Brillouin zone as well as the zone-center A 1g optical mode. This demonstrates a bond-selective approach to measuring electron-phonon coupling relevant to a broad range of photoinduced phase transitions and transient light-driven states in quantum materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Theory of photoemission from cathodes with disordered surfaces

Linear-accelerator-based applications like x-ray free electron lasers, ultrafast electron diffraction, electron beam cooling, and energy recovery linacs use photoemission-based cathodes in photoinjectors for electron sources. Most of these photocathodes are typically grown as polycrystalline materials with disordered surfaces. In order to understand the mechanism of photoemission from such cathodes and completely exploit their photoemissive properties, it is important to develop a photoemission formalism that properly describes the subtleties of these cathodes. Here, the Dowell–Schmerge (D–S) model often used to describe the properties of such cathodes gives the correct trends for photoemission properties like the quantum efficiency (QE) and the mean transverse energy (MTE) for metals; however, it is based on several unphysical assumptions. In the present work, we use Spicer’s three-step photoemission formalism to develop a photoemission model that results in the same trends for QE and MTE as the D–S model without the need for any unphysical assumptions and is applicable to defective thin-film semiconductor cathodes along with metal cathodes. As an example, we apply our model to Cs 3 Sb thin films and show that their near-threshold QE and MTE performance is largely explained by the exponentially decaying defect density of states near the valence band maximum.

43 PARTICLE ACCELERATORS↗
DOE OSTI2020

Ultrafast x-ray and electron scattering of free molecules: A comparative evaluation

Resolving gas phase molecular motions with simultaneous spatial and temporal resolution is rapidly coming within the reach of x-ray Free Electron Lasers (XFELs) and Mega-electron-Volt (MeV) electron beams. These two methods enable scattering experiments that have yielded fascinating new results, and while both are important methods for determining transient molecular structures in photochemical reactions, it is important to understand their relative merits. In the present study, we evaluate the respective scattering cross sections of the two methods and simulate their ability to determine excited state molecular structures in light of currently existing XFEL and MeV source parameters. Using the example of optically excited N-methyl morpholine and simulating the scattering patterns with shot noise, we find that the currently achievable signals are superior with x-ray scattering for equal samples and on a per-shot basis and that x-ray scattering requires fewer detected signal counts for an equal fidelity structure determination. Importantly, within the independent atom model, excellent structure determinations can be achieved for scattering vectors only to about 5 Å−1, leaving larger scattering vector ranges for investigating vibrational motions and wavepackets. Electron scattering has a comparatively higher sensitivity toward hydrogen atoms, which may point to applications where electron scattering is inherently the preferred choice, provided that excellent signals can be achieved at large scattering angles that are currently difficult to access.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Suppression of the vacuum space-charge effect in fs-photoemission by a retarding electrostatic front lens

The performance of time-resolved photoemission experiments at fs-pulsed photon sources is ultimately limited by the e–e Coulomb interaction, downgrading energy and momentum resolution. Here, we present an approach to effectively suppress space-charge artifacts in momentum microscopes and photoemission microscopes. A retarding electrostatic field generated by a special objective lens repels slow electrons, retaining the k-image of the fast photoelectrons. The suppression of space-charge effects scales with the ratio of the photoelectron velocities of fast and slow electrons. Fields in the range from -20 to 01100 V/mm for E kin = 100 eV to 4 keV direct secondaries and pump-induced slow electrons back to the sample surface. Ray tracing simulations reveal that this happens within the first 40 to 3 μm above the sample surface for E kin = 100 eV to 4 keV. An optimized front-lens design allows switching between the conventional accelerating and the new retarding mode. Time-resolved experiments at E kin = 107 eV using fs extreme ultraviolet probe pulses from the free-electron laser FLASH reveal that the width of the Fermi edge increases by just 30 meV at an incident pump fluence of 22 mJ/cm2 (retarding field -21 V/mm). For an accelerating field of +2 kV/mm and a pump fluence of only 5 mJ/cm 2 , it increases by 0.5 eV (pump wavelength 1030 nm). At the given conditions, the suppression mode permits increasing the slow-electron yield by three to four orders of magnitude. The feasibility of the method at high energies is demonstrated without a pump beam at E kin = 3830 eV using hard x rays from the storage ring PETRA III. The approach opens up a previously inaccessible regime of pump fluences for photoemission experiments.

47 OTHER INSTRUMENTATION↗
DOE OSTI2024

Nanoscale polarization transient gratings

Light manipulation at the nanoscale is essential both for fundamental science and modern technology. The quest to shorter lengthscales, however, requires the use of light wavelengths beyond the visible. In particular, in the extreme ultraviolet regime these manipulation capabilities are hampered by the lack of efficient optics, especially for polarization control. Here, we present a method to create periodic, polarization modulations at the nanoscale using a tailored configuration of the FERMI free electron laser and demonstrate its capabilities by comparing the dynamics induced by this polarization transient grating with those driven by a conventional intensity grating on a thin ferrimagnetic alloy. While the intensity grating signal is dominated by the thermoelastic response, the polarization grating excitation minimizes it, uncovering helicity-dependent responses previously undetected. We anticipate nanoscale polarization transient gratings to become useful for the study of physical, chemical and biological systems possessing chiral symmetry.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Scaling and merging time-resolved pink-beam diffraction with variational inference

Time-resolved x-ray crystallography (TR-X) at synchrotrons and free electron lasers is a promising technique for recording dynamics of molecules at atomic resolution. While experimental methods for TR-X have proliferated and matured, data analysis is often difficult. Extracting small, time-dependent changes in signal is frequently a bottleneck for practitioners. Recent work demonstrated this challenge can be addressed when merging redundant observations by a statistical technique known as variational inference (VI). However, the variational approach to time-resolved data analysis requires identification of successful hyperparameters in order to optimally extract signal. In this case study, we present a successful application of VI to time-resolved changes in an enzyme, DJ-1, upon mixing with a substrate molecule, methylglyoxal. We present a strategy to extract high signal-to-noise changes in electron density from these data. Furthermore, we conduct an ablation study, in which we systematically remove one hyperparameter at a time to demonstrate the impact of each hyperparameter choice on the success of our model. We expect this case study will serve as a practical example for how others may deploy VI in order to analyze their time-resolved diffraction data.

47 OTHER INSTRUMENTATION↗
DOE OSTI2023

Going around the Kok cycle of the water oxidation reaction with femtosecond X-ray crystallography

The water oxidation reaction in photosystem II (PS II) produces most of the molecular oxygen in the atmosphere, which sustains life on Earth, and in this process releases four electrons and four protons that drive the downstream process of CO 2 fixation in the photosynthetic apparatus. The catalytic center of PS II is an oxygen-bridged Mn 4 Ca complex (Mn 4 CaO 5 ) which is progressively oxidized upon the absorption of light by the chlorophyll of the PS II reaction center, and the accumulation of four oxidative equivalents in the catalytic center results in the oxidation of two waters to dioxygen in the last step. The recent emergence of X-ray free-electron lasers (XFELs) with intense femtosecond X-ray pulses has opened up opportunities to visualize this reaction in PS II as it proceeds through the catalytic cycle. In this review, we summarize our recent studies of the catalytic reaction in PS II by following the structural changes along the reaction pathway via room-temperature X-ray crystallography using XFELs. The evolution of the electron density changes at the Mn complex reveals notable structural changes, including the insertion of O X from a new water molecule, which disappears on completion of the reaction, implicating it in the O—O bond formation reaction. We were also able to follow the structural dynamics of the protein coordinating with the catalytic complex and of channels within the protein that are important for substrate and product transport, revealing well orchestrated conformational changes in response to the electronic changes at the Mn 4 Ca cluster.

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

Tracking structural solvent reorganization and recombination dynamics following e – photoabstraction from aqueous I – with femtosecond x-ray spectroscopy and scattering

Here we present a sub-picosecond resolved investigation of the structural solvent reorganization and geminate recombination dynamics following 400 nm two-photon excitation and photodetachment of a valence p electron from the aqueous atomic solute, I–(aq). The measurements utilized time-resolved X-ray Absorption Near Edge Structure (TR-XANES) spectroscopy and X-ray Solution Scattering (TR-XSS) at the Linac Coherent Light Source x-ray free electron laser in a laser pump/x-ray probe experiment. The XANES measurements around the L 1 -edge of the generated nascent iodine atoms (I 0 ) yield an average electron ejection distance from the iodine parent of 7.4 ± 1.5 Å with an excitation yield of about 1/3 of the 0.1M NaI aqueous solution. The kinetic traces of the XANES measurement are in agreement with a purely diffusion-driven geminate iodine–electron recombination model without the need for a long-lived (I 0 :e–) contact pair. Nonequilibrium classical molecular dynamics simulations indicate a delayed response of the caging H 2 O solvent shell and this is supported by the structural analysis of the XSS data: We identify a two-step process exhibiting a 0.1 ps delayed solvent shell reorganization time within the tight H-bond network and a 0.3 ps time constant for the mean iodine–oxygen distance changes. The results indicate that most of the reorganization can be explained classically by a transition from a hydrophilic cavity with a well-ordered first solvation shell (hydrogens pointing toward I–) to an expanded cavity around I 0 with a more random orientation of the H 2 O molecules in a broadened first solvation shell.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Ultrafast formation of domain walls of a charge density wave in SmTe 3

We study ultrafast x-ray diffraction on the charge density wave (CDW) of SmTe 3 using an x-ray free-electron laser. The high momentum and time resolution afforded by the x-ray laser enabled capturing fine wave-vector and time-dependent features of the CDW that originate from fast (in time) and sharp (in real space) variations of the CDW lattice distortion, which we attribute to an inversion of the order parameter. These domain inversions occur near the surface and are caused by the short penetration depth of the near-infrared pump with the wavelength centered at 800 nm, resulting in CDW domain walls perpendicular to the sample surface. These domain walls break the CDW long-range order on the scale of the x-ray probe depth, controlled experimentally by the x-ray incidence angle and suppress the diffraction intensity of the CDW for times much longer than the ~1–ps recovery of the electronic gap observed in time and angle-resolved photoemission spectroscopy. We model the spatial and temporal dependences of the order parameter using a simple Ginzburg-Landau model with all the parameters obtained from the published literature. We find reasonable agreement between the calculated and the measured diffraction across the momentum, time, fluence, and incidence angle dependence without adjusting any parameters. In conclusion, we reconstruct the spatial and temporal dependences of the lattice order parameter and find that at long times, depending on the pump fluence, multiple domain walls remain at distances of a few nanometers from the surface.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Ligand‐Mediated Quantum Yield Enhancement in 1‐D Silver Organothiolate Metal–Organic Chalcogenolates

X-ray free electron laser (XFEL) microcrystallography and synchrotron single-crystal crystallography are used to evaluate the role of organic substituent position on the optoelectronic properties of metal–organic chalcogenolates (MOChas). MOChas are crystalline 1D and 2D semiconducting hybrid materials that have varying optoelectronic properties depending on composition, topology, and structure. While MOChas have attracted much interest, small crystal sizes impede routine crystal structure determination. A series of constitutional isomers where the aryl thiol is functionalized by either methoxy or methyl ester are solved by small molecule serial femtosecond X-ray crystallography (smSFX) and single crystal rotational crystallography. While all the methoxy examples have a low quantum yield (0-1%), the methyl ester in the ortho position yields a high quantum yield of 22%. Here, the proximity of the oxygen atoms to the silver inorganic core correlates to a considerable enhancement of quantum yield. Four crystal structures are solved at a resolution range of 0.8–1.0 Å revealing a collapse of the 2D topology for functional groups in the 2- and 3- positions, resulting in needle-like crystals. Further analysis using density functional theory (DFT) and many-body perturbation theory (MBPT) enables the exploration of complex excitonic phenomena within easily prepared material systems.

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

Plasma-wakefield accelerator simultaneously boosts electron beam energy and brightness

High-energy particle colliders and X-ray free-electron lasers demand electron beams with qualities currently achieved only in kilometer-scale radio-frequency accelerators. Plasma accelerators promise a compact alternative but have faced challenges in delivering the needed beam quality at relevant energies. Here, we demonstrate that a plasma-wakefield accelerator operating in the nonlinear regime acts as a transformer to simultaneously boost the energy and brightness of an electron bunch injected from the plasma. Using a 10-GeV drive bunch and a three-stage meter-scale plasma source, we generated electron bunches exceeding 20 GeV with sub-percent energy spread, 2 mm·mrad normalized emittance, and multi-kA peak current. A significant number of drive-bunch electrons lost over 90% of their energy, a prerequisite for high energy-conversion efficiency. This demonstration of an energy transformer ratio exceeding two and a brightness enhancement over an order of magnitude opens a path towards cost-effective accelerators for future colliders and light sources.

experimental particle physics↗
DOE OSTI2024

Design and performance of a magnetic bottle electron spectrometer for high-energy photoelectron spectroscopy

We describe the design and performance of a magnetic bottle electron spectrometer (MBES) for high-energy electron spectroscopy. Our design features a 2 m long electron drift tube and electrostatic retardation lens, achieving sub-electronvolt (eV) electron kinetic energy resolution for high energy (several hundred eV) electrons with a close to 4π collection solid angle. A segmented anode electron detector enables the simultaneous collection of photoelectron spectra in high resolution and high collection efficiency modes. This versatile instrument is installed at the time-resolved molecular and optical sciences instrument at the Linac Coherent Light Source x-ray free-electron laser (XFEL). In this paper, we demonstrate its high resolution, collection efficiency, and spatial selectivity in measurements where it is coupled to an XFEL source. These combined characteristics are designed to enable high-resolution time-resolved measurements using x-ray photoelectron, absorption, and Auger–Meitner spectroscopy. We also describe the pervasive artifact in MBES time-of-flight spectra that arises from a periodic modulation in electron collection efficiency and present a robust analysis procedure for its removal.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2025

Shake-Down Spectroscopy as State- and Site-Specific Probe of Ultrafast Chemical Dynamics

Tracking the multifarious ultrafast electronic and structural changes occurring in a molecule during a photochemical transformation is a challenging endeavor that benefits from recent experimental and computational progress in time-resolved techniques. Measurements of valence electronic states, which provide a global picture of the bonding structure of the molecule, and core electronic states, which provide insight into the local environment, traditionally require different approaches and are often studied separately. Here, we demonstrate that X-ray pulses from a seeded free-electron laser (FEL) enable the measurement of high-resolution, time-resolved X-ray photoelectron spectra (XPS) that capture weak satellite states resulting from shake-down processes in a valence-excited molecule. This approach effectively combines the advantages of both valence- and core-state investigations. We applied this method to investigate photoexcited CS2 molecules, where the role of internal conversion (IC) and intersystem crossing (ISC) in determining the predissociation dynamics is controversial. We present XPS spectra from photoexcited CS2, obtained at the FERMI FEL. High-resolution measurements, compared to the corresponding spectra obtained from accurate multireference quantum chemical calculations, reveal that shake-down satellite channels are highly sensitive to both valence electronic and geometric changes. Previous studies of the predissociation dynamics have led to uncertain assignments of the branching between singlet and triplet excited states. We derive a propensity rule that demonstrates the spin-selectivity of the shake-downs. This selectivity allows us to unequivocally assign contributions from the bright and dark singlet excited states, with populations tracked along the predissociation dynamic pathway.

Thompson, Henry J. [Univ. of Southampton (United K↗