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At least 307 records · Page 17

Measurement of interfacial thermal resistance in high-energy-density matter

Heat transport across interfaces is a ubiquitous phenomenon with many unresolved aspects. In particular, it is unknown if an interfacial thermal resistance (ITR) occurs in matter with high-energy-density where free electrons dominate the heat conduction. Here, we report on the first experimental evidence that a significant heat barrier is present between two different regions of high-energy-density matter: a strongly heated tungsten wire and a surrounding plastic layer that stays relatively cold. We use diffraction-enhanced imaging to track the time evolution of density discontinuities and reconstruct the temperature evolution in the quasi-stationary stage. The clear signatures of a temperature jump demonstrate the importance of the ITR for strongly heated systems with far-reaching implications for interpreting experiments and applications like inertial confinement fusion.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Time-resolved X-ray imaging of the current filamentation instability in solid-density plasmas

The streaming of energetic charged particles can magnetize astrophysical and laboratory plasmas via the current filamentation instability. Despite its importance, the experimental characterization of this instability has remained a challenge. Here, we report an experiment combining a high-intensity optical laser with a high-brightness X-ray free electron laser that successfully images the instability in solid-density plasmas with 200 nm spatial and 50 fs temporal resolution. We characterize the development of μm-scale filamentary structures and their evolution over tens of picoseconds through a non-linear merging process. The measured plasma density modulations and long merging time reveal the critical importance of space-charge effects and ion motion on this electron-driven instability. Supporting theoretical analysis and kinetic simulations help distinguish the relative role of space-charge and resistive effects. Our findings indicate that magnetic fields on the order of 10 megagauss are produced, with important implications for transport and radiation emission of energetic particles in plasmas.

Schoenwaelder, Christopher [SLAC National Accelera↗

Chemical crystallography by serial femtosecond X-ray diffraction

Abstract Inorganic–organic hybrid materials represent a large share of newly reported structures, owing to their simple synthetic routes and customizable properties 1 . This proliferation has led to a characterization bottleneck: many hybrid materials are obligate microcrystals with low symmetry and severe radiation sensitivity, interfering with the standard techniques of single-crystal X-ray diffraction 2,3 and electron microdiffraction 4–11 . Here we demonstrate small-molecule serial femtosecond X-ray crystallography (smSFX) for the determination of material crystal structures from microcrystals. We subjected microcrystalline suspensions to X-ray free-electron laser radiation 12,13 and obtained thousands of randomly oriented diffraction patterns. We determined unit cells by aggregating spot-finding results into high-resolution powder diffractograms. After indexing the sparse serial patterns by a graph theory approach 14 , the resulting datasets can be solved and refined using standard tools for single-crystal diffraction data 15–17 . We describe the ab initio structure solutions of mithrene (AgSePh) 18–20 , thiorene (AgSPh) and tethrene (AgTePh), of which the latter two were previously unknown structures. In thiorene, we identify a geometric change in the silver–silver bonding network that is linked to its divergent optoelectronic properties 20 . We demonstrate that smSFX can be applied as a general technique for structure determination of beam-sensitive microcrystalline materials at near-ambient temperature and pressure.

36 MATERIALS SCIENCE↗

X-ray microscopy and talbot imaging with the matter in extreme conditions X-ray imager at LCLS

The last decade has shown the great potential that X-ray Free Electron Lasers (FEL) have to study High Energy Density (HED) physics. Experiments at FELs have made significant breakthroughs in Shock Physics and Dynamic Diffraction, Dense Plasma Physics and Warm Dense Matter Science, using techniques such as isochoric heating, inelastic scattering, small angle scattering and X-ray diffraction. In addition, and complementary to these techniques, the coherent properties of the FEL beam can be used to image HED samples with high fidelity. We present new imaging diagnostics and techniques developed at the Matter in Extreme Conditions (MEC) instrument at Linac Coherent Light Source (LCLS) over the last few years. We show results in Phase Contrast Imaging geometry, where the X-ray beam propagates from the target to a camera revealing its phase, as well as in Direct Imaging geometry, where a real image of the sample plane is produced in the camera with a spatial resolution down to 200 nm. Last, we show an implementation of the Talbot Imaging method allowing both X-ray phase and intensity measurements change introduced by a target with sub-micron resolution.

47 OTHER INSTRUMENTATION↗

All hard X-ray transient grating spectroscopy

Optical-domain transient grating (TG) spectroscopy is the ideal tool to investigate transport phenomena in gases, liquids and solids, but it is limited to typically micron-size grating periods. Extreme-Ultraviolet TG has represented a major leap forward to access the mesoscopic scales. Hard X-ray TGs open access in principle to the nanoscale. Hard X-ray TGs were recently generated using the Talbot effect and probed by optical pulses, but these hinder exploiting the advantages of the nanoscale gratings. Here, we present an all-X-ray TG study, in which few-femtosecond hard X-ray pulses are used both for excitation and probing. Our experiment was performed on an amorphous film of an FeGd alloy and on a thin silicon single crystal. The results show a manifestation of the TG induced by the X-ray pump and probe pulses in the form of Talbot carpets, as well as temporal evolution of the grating in crystalline silicon showing coherent optical phonons. Ultrafast all-X-ray TG spectroscopy has the potential to study fundamental excitations with femtosecond time resolution and nanometer spatial sensitivity.

Ferrari, Eugenio [Deutsches Elektronen-Synchrotron↗

Elucidating Norrish type I reactive pathways by ultrafast X-ray absorption spectroscopy

Norrish type I reactions selectively cleave carbon–carbon bonds directly adjacent to carbonyl groups. Despite their broad use in combination with aromatic carbonyls for additive manufacturing and dental UV curing applications, the nature of the photochemically active state and its population mechanism remain insufficiently understood. Detailed mechanistic insight requires mapping of the photoexcited population flow involving internal conversion and intersystem crossing. We present a time-domain study of gas phase acetophenone as a prototypical aromatic carbonyl combining soft X-ray time-resolved near-edge X-ray absorption fine structure (TR-NEXAFS) spectroscopy at the oxygen K-edge with ab initio multiple spawning (AIMS) simulations. Exploiting the specific sensitivity of TR-NEXAFS spectroscopy to states with nπ* character, we observe population transfer from the initially excited 1 ππ* state to the 1 nπ* state with a time constant of (0.13 ± 0.02) ps after an initial induction period of (0.12 ± 0.02) ps without population transfer, in quantitative agreement with the AIMS simulations. The population in the 1 nπ* state subsequently decays via intersystem crossing, likely mediated by a 3 ππ* state, within (3.17 ± 0.66) ps to a long-lived 3 nπ* state, which is presumed to be active towards Norrish type I chemistry.

Graßl, Martin [SLAC National Accelerator Laborator↗

Model-free Rayleigh weight from x-ray Thomson scattering measurements

X-ray Thomson scattering (XRTS) has emerged as a powerful tool for the diagnostics of matter under extreme conditions. In principle, it gives one access to important system parameters such as the temperature, density, and ionization state, but the interpretation of the measured XRTS intensity usually relies on theoretical models and approximations. In this context, a key property is given by the Rayleigh weight that describes the electronic localization around the ions. Here, we show that it is possible to extract the Rayleigh weight directly from the experimental data without the need for any model calculations or simulations. As a practical application, we consider an experimental measurement of strongly compressed Be at the National Ignition Facility [Döppner et al., Nature 618, 270–275 (2023)]. We demonstrate that experimental results for the Rayleigh weight open up new avenues for the interpretation of XRTS experiments by matching the measurement with ab initio simulations such as density functional theory or path integral Monte Carlo. Interestingly, this new procedure leads to significantly lower density compared to previously used chemical models.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Imaging the photochemistry of cyclobutanone using ultrafast electron diffraction: Experimental results

We investigated the ultrafast structural dynamics of cyclobutanone following photoexcitation at λ = 200 nm using gas-phase megaelectronvolt ultrafast electron diffraction. Our investigation complements the simulation studies of the same process within this special issue. It provides information about both electronic state population and structural dynamics through well-separable inelastic and elastic electron scattering signatures. We observe the depopulation of the photoexcited S 2 state of cyclobutanone with n3s Rydberg character through its inelastic electron scattering signature with a time constant of (0.29 ± 0.2) ps toward the S 1 state. The S 1 state population undergoes ring-opening via a Norrish Type-I reaction, likely while passing through a conical intersection with S 0 . The corresponding structural changes can be tracked by elastic electron scattering signatures. These changes appear with a delay of (0.14 ± 0.05) ps with respect to the initial photoexcitation, which is less than the S 2 depopulation time constant. This behavior provides evidence for the ballistic nature of the ring-opening once the S 1 state is reached. The resulting biradical species react further within (1.2 ± 0.2) ps via two rival fragmentation channels yielding ketene and ethylene, or propene and carbon monoxide. Furthermore, our study showcases the value of both gas-phase ultrafast diffraction studies as an experimental benchmark for nonadiabatic dynamics simulation methods and the limits in the interpretation of such experimental data without comparison with such simulations.

Carbon monoxide↗

Shock propagation in aerogel and TPP foams for inertial fusion energy target design

Achieving practical inertial fusion energy (IFE) requires the development of target designs with well-characterized microstructure and compression response. We measured shock dynamics in low-density (17.5–500 mg/cm 3 ) aerogel and two-photon polymerization (TPP) foams using x-ray phase contrast imaging (XPCI) methods and the Velocity Interferometer System for Any Reflector. By analyzing shock front evolution, we examined how target type and density influence shock propagation and energy dissipation. Talbot-XPCI shows that aerogels support a smooth, bowed shock front due to their homogeneous nanometer-scale pore network. In contrast, TPP foams exhibit irregular, stepwise propagation driven by interactions with their periodic micrometer-scale lattice. Shock velocity follows a power-law relation: aerogels deviate from classical ρ −1/2 scaling due to pore-collapse dissipation, while TPP foams follow the trend with larger uncertainties from density variations. Comparisons with xRAGE simulations reveal systematic underestimation of shock speeds. These results provide the first experimental constraints on shock propagation in TPP foams over a wide density range and highlight the influence of internal structure on anisotropic shock behavior. Our findings support improved benchmarking of EOS and hydrodynamic models and inform the design of foam architectures that promote implosion symmetry in IFE capsules.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Ultrafast x-ray scattering of photodissociation dynamics in 2-iodothiophene

Here, a time-resolved x-ray scattering (TRXS) investigation of the photodissociation dynamics of gas-phase 2-iodothiophene molecules following 252 nm excitation is presented. Structural evolution of the molecule and dynamical information on the resulting photofragments were captured using femtosecond x-ray free-electron laser pulses. Two dissociation pathways were identified, arising via excitation to ππ* and (n/π)σ* states, respectively, yielding distinct interfragment recoil velocities of ∼6.4 Åps −1 and 17.0 Åps −1 . A comparison of asymptotic scattering data with simulated patterns indicates that the thiophene ring remains closed following dissociation at this wavelength. Modeling the experimental data yields a branching ratio of ∼3:1 in favor of the high velocity channel. These findings demonstrate the capability of TRXS to disentangle concurrent ultrafast reaction pathways and provide detailed structural insight into energy redistribution during photoinduced bond fission in complex molecular systems.

Razmus, Weronika O. [Univ. of Southampton (United ↗

Spectral deconvolution without the deconvolution: Extracting temperature from x-ray Thomson scattering spectra without the source-and-instrument function

X-ray Thomson scattering (XRTS) probes the dynamic structure factor of the system, but the measured spectrum is broadened by the combined source-and-instrument function (SIF) of the setup. In order to extract properties such as temperature from an XRTS spectrum, the broadening by the SIF needs to be removed. Recent work [Dornheim et al. Nat. Commun. 13 , 7911 (2022)] has suggested that the SIF may be deconvolved using the two-sided Laplace transform. However, the extracted information can depend strongly on the shape of the input SIF, and the SIF is in practice challenging to measure accurately. Here, we propose an alternative approach: we demonstrate that considering ratios of Laplace-transformed XRTS spectra collected at different scattering angles is equivalent to performing the deconvolution, but without the need for explicit knowledge of the SIF. From these ratios, it is possible to directly extract the temperature from the scattering spectra, when the system is in thermal equilibrium. We find the method to be generally robust to spectral noise and physical differences between the spectrometers, and we explore situations in which the method breaks down. Furthermore, the fact that consistent temperatures can be extracted for systems in thermal equilibrium indicates that non-equilibrium effects could be identified by inconsistent temperatures of a few eV between the ratios of three or more scattering angles.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

In situ X-ray diffraction of silicate liquids and glasses under dynamic and static compression to megabar pressures

Properties of liquid silicates under high-pressure and high-temperature conditions are critical for modeling the dynamics and solidification mechanisms of the magma ocean in the early Earth, as well as for constraining entrainment of melts in the mantle and in the present-day core–mantle boundary. In this paper, we present in situ structural measurements by X-ray diffraction of selected amorphous silicates compressed statically in diamond anvil cells (up to 157 GPa at room temperature) or dynamically by laser-generated shock compression (up to 130 GPa and 6,000 K along the MgSiO 3 glass Hugoniot). The X-ray diffraction patterns of silicate glasses and liquids reveal similar characteristics over a wide pressure and temperature range. Beyond the increase in Si coordination observed at 20 GPa, we find no evidence for major structural changes occurring in the silicate melts studied up to pressures and temperatures exceeding Earth’s core mantle boundary conditions. This result is supported by molecular dynamics calculations. Our findings reinforce the widely used assumption that the silicate glasses studies are appropriate structural analogs for understanding the atomic arrangement of silicate liquids at these high pressures.

58 GEOSCIENCES↗

Brighter, faster, stronger: ultrafast scattering of free molecules

Advances in FEL technologies have contributed remarkably to various scientific fields over the past decade, and ultrafast molecular dynamics is no exception. The ability to probe motions of the molecule via scattering provides uniquely direct structural information, which, when combined with traditional spectroscopic techniques of comparable temporal resolution, paints a holistic movie of the molecular dynamics. This review aims to provide an introduction to the ultrafast scattering of gas-phase molecules, and to identify the key results and technological breakthroughs that advance our acquaintance of ultrafast molecular dynamics, with a particular focus on the achievements in ultrafast molecular dynamics since the first generation of FEL facilities. We pre- sent a brief history of gas-phase ultrafast scattering and the fundamentals of electron- and x-ray scattering, highlighting the complementarity, differences, and bottlenecks of the two experimental scattering methods. Furthermore, we then consider key upgrades in XRS and UED experiments that facilitated the unprecedented spatiotemporal resolution that enabled many of the notable results in the field. Finally, we examine anticipated facility upgrades that address the demand for experimental versatility and enable further developments and exploration.

74 ATOMIC AND MOLECULAR PHYSICS↗

On ultrafast x-ray scattering methods for magnetism

With the introduction of x-ray free electron laser sources around the world, new scientific approaches for visualizing matter at fundamental length and time-scales have become possible. As it relates to magnetism and ‘magnetic-type’ systems, advanced methods are being developed for studying ultrafast magnetic responses on the time-scales at which they occur. We describe three capabilities which have the potential to seed new directions in this area and present original results from each: pump-probe x-ray scattering with low energy excitation, x-ray photon fluctuation spectroscopy, and ultrafast diffuse x-ray scattering. By combining these experimental techniques with advanced modeling together with machine learning, we describe how the combination of these domains allows for a new understanding in the field of magnetism. Finally, we give an outlook for future areas of investigation and the newly developed instruments which will take us there.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Measuring dynamics of differentially rotating, unmagnetized, free-boundary plasma produced by soft x-ray irradiation

We present results from a new experiment, fielded on the MAGPIE pulsed power generator, producing a rotating, boundary-free plasma with no pre-imposed magnetic field. Angular momentum is introduced to the rotating system by the oblique collision of multiple plasma flows, which are driven by x-ray ablation of solid targets using the soft x-rays emitted from the implosion of wire array z-pinches. This produces a hydrodynamically stable plasma which undergoes ~2-3 rotations over the duration of the experiment, significantly more than previous pulsed-power platforms. Estimating the angular frequency from the electron density profile in the inner part of the rotating plasma shows that it has a quasi-Keplerian rotation profile. The system also allows for the addition of a controllable magnetic field. This, combined with the sufficiently large Reynolds (~10 5 ) and magnetic Reynolds (~10) numbers, will enable investigation of the effect of magnetic field on the structure and stability of the rotating plasma.

Physics - Plasma physics↗

Probing shock dynamics inside micro-wire targets after high-intensity laser irradiation using small angle x-ray scattering of a free-electron laser

In this paper, we present an experiment that explores the plasma dynamics of a 7μm diameter carbon wire after being irradiated with a near-relativistic-intensity short pulse laser. Using an x-ray free electron laser pulse to measure the small angle x-ray scattering signal, we observe that the scattering surface is bent and prone to instability over tens of picoseconds. The dynamics of this process are consistent with the presence of a sharp, propagating shock front inside the wire, moving at a speed close to the hole boring velocity or that expected from a thermal shock at a few tens of Mbar.

47 OTHER INSTRUMENTATION↗

Passive Freeze-Out of the Richtmyer-Meshkov Instability

The Richtmyer-Meshkov instability (RMI) poses a major challenge in inertial confinement fusion (ICF) due to its role in mixing and performance degradation. We report the first experimental observation of passive freeze-out of RMI in a low-pressure surrogate regime, an instability stagnation effect induced without modifying the driving pressure pulse or the target surface geometry. Using additively manufactured subsurface voids in a sinusoidal target, we convert a single shock into a sequence of weaker shocks that suppress instability growth upstream of the surface by over 70%. High-speed x-ray imaging and hydrodynamic simulations suggest that this suppression arises primarily from temporal shaping, with lesser contributions from spatial curvature and shock weakening. Our results demonstrate a driver-independent pathway for controlling shock-driven hydrodynamic instabilities relevant to ICF and other high energy density systems.

Materials science↗

Imaging Valence Electron Rearrangement in a Chemical Reaction Using Hard X-Ray Scattering

We have observed the signatures of valence electron rearrangement in photoexcited ammonia using ultrafast hard x-ray scattering. Time-resolved x-ray scattering is a powerful tool for imaging structural dynamics in molecules because of the strong scattering from the core electrons localized near each nucleus. Such core-electron contributions generally dominate the differential scattering signal, masking any signatures of rearrangement in the chemically important valence electrons. Ammonia represents an exception to the typically high core-to-valence electron ratio. Here, we measured 9.8 keV x-ray scattering from gas-phase deuterated ammonia following photoexcitation via a 200 nm pump pulse to the 3s Rydberg state. We observed changes in the recorded scattering patterns due to the initial photoexcitation and subsequent deuterium dissociation. Ab initio calculations confirm that the observed signal is sensitive to the rearrangement of the single photoexcited valence electron as well as the interplay between adiabatic and nonadiabatic dissociation channels. The use of ultrafast hard x-ray scattering to image the structural rearrangement of single valence electrons constitutes an important advance in tracking valence electronic structure in photoexcited atoms and molecules.

Gabalski, Ian [SLAC National Accelerator Laborator↗