A new class of focusing crystal shapes for Bragg spectroscopy of small, point-like, x-ray sources in laser produced plasmas
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Physics - Plasma physics↗
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Bragg curve spectroscopy for improved fission fragment identification
We report on the development of Bragg curve spectroscopy techniques to improve fission fragment identification in the measurement of independent fission product yields. The NIFFTE collaboration’s fissionTPC detector provides ionization energy and particle tracking information from neutroninduced fission targets. A joint effort between PNNL, LLNL, LANL, and the Colorado School of Mines is investigating the ionization profiles deposited by U-235, U-238, and Pu-239 fission products in this detector, with the goal of including additional stopping power information beyond a standard 2E analysis. The aim is to improve the determination of fragment atomic and mass numbers with this information, via methods such as parametric fits and machine learning techniques.
Fulsom, Bryan G.↗
Machine learning methods for fission product identification from Bragg curves
A fission time projection chamber (fission-TPC) was developed to provide precise neutron-induced fission measurements for several major actinides. As fission fragments lose energy in one of the gas volumes of the fission-TPC, energy loss information is captured and may be used to determine fission product yields as the stopping power of an ion is dependent on the atomic number. The work presented here demonstrates the ability to apply machine learning techniques for Bragg curve classification. A set of one million energy loss curves for 24 different fission-fragment elements was generated using common stopping power software. A ResNet architecture optimized for 1D data was used to train, test, and validate a model for light and heavy fission fragments using the simulated data. The resultant classification accuracy for the light and heavy fragments indicates that this could be a viable method for elemental classification of data from the fission-TPC.
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
Dielectronic satellite emission from a solid-density Mg plasma: Relationship to models of ionization potential depression
Here, we report on experiments where solid-density Mg plasmas are created by heating with the focused output of the Linac Coherent Light Source x-ray free-electron laser. We study the K-shell emission from the helium- and lithium-like ions using Bragg crystal spectroscopy. Observation of the dielectronic satellites in lithium-like ions confirms that the M-shell electrons appear bound for these high charge states. An analysis of the intensity of these satellites indicates that when modeled with an atomic-kinetics code, the ionization potential depression model employed needs to produce depressions for these ions which lie between those predicted by the well known Stewart-Pyatt and Ecker-Kroll models. These results are largely consistent with recent density functional theory calculations.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Solid-Density Ion Temperature from Redshifted and Double-Peaked Stark Line Shapes
Heβ spectral line shapes are important for diagnosing temperature and density in many dense plasmas. This work presents Heβ line shapes measured with high spectral resolution from solid-density plasmas with minimized gradients. The line shapes show hallmark features of Stark broadening, including quantifiable redshifts and double-peaked structure with a significant dip between the peaks; these features are compared to models through a Markov chain Monte Carlo framework. Line shape theory using the dipole approximation can fit the width and peak separation of measured line shapes, but it cannot resolve an ambiguity between electron density n e and ion temperature T i , since both parameters influence the strength of quasistatic ion microfields. Here a line shape model employing a full Coulomb interaction for the electron broadening computes self-consistent line widths and redshifts through the monopole term; redshifts have different dependence on plasma parameters and thus resolve the n e – T i ambiguity. The measured line shapes indicate densities that are 80–100% of solid, identifying a regime of highly ionized but well-tamped plasma. This analysis also provides the first strong evidence that dense ions and electrons are not in thermal equilibrium, despite equilibration times much shorter than the duration of x-ray emission; cooler ions may arise from nonclassical thermalization rates or anomalous energy transport. Furthermore, the experimental platform and diagnostic technique constitute a promising new approach for studying ion-electron equilibration in dense plasmas.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Ablating Ion Velocity Distributions in Short-Pulse-Heated Solids via X-Ray Doppler Shifts
Solids ablate under laser irradiation, but experiments have not previously characterized the initiation of this process at ultrarelativistic laser intensities. Here, we present first measurements of bulk ion velocity distributions as ablation begins, captured as a function of depth via Doppler-shifted x-ray line emission from two viewing angles. Bayesian analysis indicates that bulk ions are either nearly stationary or flowing outward at the plasma sound speed. The measurements quantitatively constrain the laser-plasma ablation mechanism, suggesting that a steplike electrostatic potential structure drives solid disassembly.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Determination of Thermal Damage Threshold in THz Photomixers Using Raman Spectroscopy
The increase of device lifetime and reliability of THz photomixers will play an essential role in their possible future application. Therefore, their optimal work conditions/operation range, i.e., the maximal incident optical power should be experimentally estimated. We fabricated and tested THz photomixer devices based on nitrogen-implanted GaAs integrated with a Bragg reflector. Raman spectroscopy was applied to investigate the material properties and to disclose any reversible or irreversible material changes. The results indicate that degradation effects in the photomixer structures/material could be avoided if the total optical power density does not exceed levels of about 0.7 mW/µm 2 for 100 min of operation. Furthermore, the investigations performed during 1000 min of optical exposure on the photomixer devices’ central region comprising interdigitated metal-semiconductor-metal (MSM) structures suggest a reversible “curing” mechanism if the power density level of ~0.58 mW/µm 2 is not exceeded. Long-term operation (up to 1000 h) reveals that the photomixer structures can withstand an average optical power density of up to ~0.4 mW/µm 2 without degradation when biased at 10 V. Besides the decrease of the position of the A1g (LO) Raman mode from ~291 cm -1 down to ~288 cm -1 with increasing optical power density and operation time, broad Raman modes evolve at about 210 cm -1 , which can be attributed to degradation effects in the active photomixer/MSM area. In addition, the performed carrier lifetime and photomixer experiments demonstrated that these structures generated continuous wave sub-THz radiation efficiently as long as their optimal work conditions/operation range were within the limits established by our Raman studies.
36 MATERIALS SCIENCE↗
Dispersive X-ray absorption spectroscopy using independent grazing-incidence focusing and convexly bent Bragg-crystal dispersing optics
We present a modular instrument for dispersive X-ray absorption spectroscopy (DXAS) developed for the Advanced Spectroscopy Beamline at Sector 25 of the Advanced Photon Source. The setup employs a double-multilayer monochromator to provide X-rays with a broad energy bandwidth, Kirkpatrick–Baez mirrors for focusing, a convexly bent Bragg-crystal polychromator for energy dispersion, and a pixel-array detector to resolve all X-ray energies and collect their intensity simultaneously, thereby enabling acquisition of a full X-ray absorption spectrum in a single shot. The use of separate optics for X-ray focusing and energy dispersion provides high spatial resolution and avoids chromatic aberrations inherent in focusing bent-crystal optics, and a modular design makes implementation of the technique at other beamlines possible without requiring modifications to the upstream beamline configurations. Theoretical calculations are performed to determine optimal instrument operating parameters and demonstrate that an energy resolution better than the K-edge core-hole lifetime broadening can be maintained while providing a sufficient bandwidth for X-ray absorption near-edge structure spectroscopy through the full operating range of 5–11 keV. Additionally, instrument design, data analysis methods, and initial DXAS results on lithium–manganese–nickel oxide laminates are presented.
47 OTHER INSTRUMENTATION↗
Iterative Bragg peak removal on X-ray absorption spectra with automatic intensity correction
This study introduces a novel iterative Bragg peak removal with automatic intensity correction (IBR-AIC) methodology for X-ray absorption spectroscopy (XAS), specifically addressing the challenge of Bragg peak interference in the analysis of crystalline materials. The approach integrates experimental adjustments and sophisticated post-processing, including an iterative algorithm for robust calculation of the scaling factor of the absorption coefficients and efficient elimination of the Bragg peaks, a common obstacle in accurately interpreting XAS data, particularly in crystalline samples. The method was thoroughly evaluated on dilute catalysts and thin films, with fluorescence mode and large-angle rotation. The results underscore the technique's effectiveness, adaptability and substantial potential in improving the precision of XAS data analysis. While demonstrating significant promise, the method does have limitations related to signal-to-noise ratio sensitivity and the necessity for meticulous angle selection during experimentation. Overall, IBR-AIC represents a significant advancement in XAS, offering a pragmatic solution to Bragg peak contamination challenges, thereby expanding the applications of XAS in understanding complex materials under diverse experimental conditions.
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
Near total reflection x-ray photoelectron spectroscopy: quantifying chemistry at solid/liquid and solid/solid interfaces
Near total reflection regime has been widely used in x-ray science, specifically in grazing incidence small angle x-ray scattering and in hard x-ray photoelectron spectroscopy (XPS). In this work, we introduce some practical aspects of using near total reflection (NTR) in ambient pressure XPS and apply this technique to study chemical concentration gradients in a substrate/photoresist system. Experimental data are accompanied by x-ray optical and photoemission simulations to quantitatively probe the photoresist and the interface with the depth accuracy of ~1 nm. Together, our calculations and experiments confirm that NTR XPS is a suitable method to extract information from buried interfaces with highest depth-resolution, which can help address open research questions regarding our understanding of concentration profiles, electrical gradients, and charge transfer phenomena at such interfaces. Furthermore, the presented methodology is especially attractive for solid/liquid interface studies, since it provides all the strengths of a Bragg-reflection standing-wave spectroscopy without the need of an artificial multilayer mirror serving as a standing wave generator, thus dramatically simplifying the sample synthesis.
solid/solid interface↗
Dynamic Nanoscale Spatial Heterogeneity in a Perovskite-to-Brownmillerite Topotactic Phase Transformation
Phase transitions are omnipresent in modern condensed matter physics and its applications. In solids, first-order phase transformations typically occur by nucleation and growth under nonequilibrium conditions. Under constant external conditions, e.g., constant annealing temperature and pressure, the nucleation and growth dynamics are often thought of as spatially and temporally independent. Here, in situ Bragg X-ray photon correlation spectroscopy (XPCS) reveals nanoscale spatial and dynamical heterogeneity in the perovskite-to-brownmillerite topotactic phase transformation in La 0.7 Sr 0.3 CoO 3 thin films annealed under constant reducing conditions over a time span of multiple hours. Specifically, a time scale associated with domain growth remains stable, with a corresponding domain wall speed of v d = 6 ± 0.5 × 10 –4 nm/s (2 ± 0.2 nm/h), while a slower time scale, associated with temperature-driven depinning of domains, leads to accelerating dynamics with time scales following an aging power law with exponent −2.2 ± 0.5. This experiment demonstrates that Bragg XPCS is a powerful tool to study nanoscale dynamics in structural phase transformations, with the ability to extract quantitative average values related to nanodomain motion in situ. Furthermore, the results are relevant for phase engineering of phase-change devices, as they show that nanoscale dynamics, linked to domain and domain-wall motion, can continuously evolve and speed up with time, even hours after the initiation of the phase transformation, with potential repercussions on electrical performance.
X-ray photon correlation spectroscopy↗
Hard x-ray standing-wave photoemission study of the interfaces in a BiFeO$_3$/La$_{0.7}$Sr$_{0.3}$MnO$_3$ superlattice
Hybrid multiferroics such as BiFeO$_3$ (BFO) and La$_{0.7}$Sr$_{0.3}$MnO$_3$ (LSMO) heterostructures are highly interesting functional systems due to their complex electronic and magnetic properties. One of the key parameters influencing the emergent properties is the quality of interfaces, where varying interdiffusion lengths can give rise to different chemistry and distinctive electronic states. Here we report high-resolution depth resolved chemical and electronic investigation of BFO/LSMO superlattice using standing-wave hard X-ray photoemission spectroscopy in the first-order Bragg as well as near-total-reflection geometry. Our results show that the interfaces of BFO on top of LSMO are atomically abrupt, while the LSMO on top of BFO interfaces show an interdiffusion length of around 1.2 unit cells. The two interfaces also exhibit different chemical gradients, with the BFO/LSMO interface being Sr-terminated by a spectroscopically distinctive high binding energy component in Sr 2p core-level spectra, which is spatially contained within 1 unit cell from the interface. From the electronic point of view, unique valence band features were observed for bulk-BFO, bulk-LSMO and their interfaces. Our X-ray optical analysis revealed a unique electronic signature at the BFO/LSMO interface, which we attribute to the coupling between those respective layers. Valence band decomposition based on the Bragg-reflection standing-wave measurement also revealed the band alignment between BFO and LSMO layers. Our work demonstrates that standing-wave hard x-ray photoemission is a reliable non-destructive technique for probing depth-resolved electronic structure of buried layers and interfaces with sub-unit-cell resolution. Equivalent investigations can be successfully applied to a broad class of material such as perovskite complex oxides with emergent interfacial phenomena.
Martins, HP↗
Quantification of Oxygen Vacancies in SrFe0.5Cr0.5O3−δ Thin Films: Correlating Lattice Expansion with Oxidation State Variability
Oxygen vacancies (VO), even in the dilute regime, can significantly impact the physical and chemical properties of complex oxides. It is however challenging to reliably detect and adequately quantify such defects in thin film samples where the VO concentration and distribution may further vary in response to interfacial strain. Here, we present a method to quantify VO concentrations in SrFe0.5Cr0.5O3−δ (SFCO) epitaxial thin films. Through coherent Bragg rod analysis, X-ray absorption spectroscopy, and theoretical modeling, we systematically correlate the c-axis lattice expansion detected in SFCO films with a VO concentration gradient. Our results reveal a nearly linear relationship between oxygen off-stoichiometry and out-of-plane lattice expansion in coherently strained SFCO films, with δ increasing from 0.32 to 0.52 and the lattice expanding by ∼1.0%. Moreover, a significant decrease in Cr oxidation state (from Cr5+ to Cr3+) is observed as the VO concentration increases, while the Fe oxidation state remains fixed at Fe3+. Our findings provide a reliable way to quantify oxygen stoichiometry in complex oxides, offering a pathway to design materials with precisely tailored structure–property relationships.
Hossain, Mohammad Delower↗
Dynamics of Thermally Driven Domain Transformation in Ferroelectric Thin Films
An important feature in ultrathin ferroelectric films is the spontaneous formation of nanoscale polarization domain patterns. Epitaxial strain can greatly increase the ferroelectric transition temperature such that films can be in the ferroelectric state during growth. On the other hand, depolarization fields compete with ferroelectricity in ultrathin films, and, consequently, the optimal domain configuration during growth is a moving target. Under these conditions it is readily possible for a grown film to be in a nonequilibrium domain configuration. As the energy landscape in the system is quite complex, the relaxation dynamics by which a system can evolve towards the true equilibrium configuration are also quite interesting. Here, to capture the details of this process we used Bragg-geometry x-ray photon correlation spectroscopy (XPCS), in which x-ray scattering speckle patterns contain the information from the domain arrangements inside the film. With modest heating (∼150 °C) domain relaxation from 𝑇 (tetragonal) to 𝑀 𝐶 (monoclinic) was observed in BaTiO 3 films grown on ultrathin ferroelectric PbTiO 3 layers. Two-time correlation analysis reveals fascinating details associated with sticking points and reversals in the process.
36 MATERIALS SCIENCE↗
All-dielectric multi-resonant bullseye antennas
Integrated devices that generate multiple optical resonances in the same volume can enhance on-chip nonlinear frequency generation, nonlinear spectroscopy, and quantum sensing. Here, we demonstrate circular Bragg antennas that exhibit multiple spatially overlapping, polarization-selective optical resonances. Using templated atomic layer deposition of TiO 2 , these devices can be fabricated on arbitrary substrates, making them compatible with a wide range of nonlinear materials and sensing targets, and couple efficiently to underlying films. In this work, we detail the design, simulation, and fabrication of all-dielectric multi-resonant bullseye antennas and characterize their performance using polarized broadband reflection spectroscopy.
47 OTHER INSTRUMENTATION↗
Manipulating Ferroelectric Topological Polar Structures with Twisted Light
Abstract The dynamic control of non‐equilibrium states represents a central challenge in condensed matter physics. While intense terahertz fields drive metal‐insulator transitions and ferroelectricity via soft phonon modes, recent theory suggests that twisted light with orbital angular momentum (OAM) offers a distinct route to manipulate ferroelectric order and stabilize topological excitations including skyrmions, vortices, and Hopfions. Control of ferroelectric polarization in quasi‐2D CsBiNb 2 O 7 (CBNO) is demonstrated using non‐resonant twisted ultra‐violet (UV) light (375 nm, 800 THz). Combining in situ X‐ray Bragg coherent diffractive imaging (BCDI), twisted optical Raman spectroscopy, and density functional theory (DFT), three‐dimensional (3D) ionic displacements, strain fields, and polarization changes are resolved in single crystals. Operando measurements reveal light‐induced strain hysteresis under twisted light–a hallmark of nonlinear, history‐dependent ferroelastic switching driven by OAM. Discrete, irreversible domain transitions emerge as the topological charge ℓ is cycled, stabilizing non‐trivial domain textures including vortex‐antivortex pairs, Bloch/anti‐Bloch points, and merons. These persist after OAM removal, indicating a memory effect. Competing mechanisms are discussed, including multiphoton absorption, strain‐mediated polarization switching, and defect‐wall interactions. The findings establish structured light as a tool for deterministic, reversible control of ferroic states, enabling optically reconfigurable non‐volatile devices.
Chemistry↗
Interplay between Cation “Coloring” and Stereochemically Active Lone Pairs in AgBiS 2 Thin Films
Solution-processed AgBiS 2 thin films were fabricated using novel thiol− amine precursor inks to investigate the stereochemical activity of Bi 3+ 6s 2 lone pairs and their impact on the structure. A dual-space analysis combining Bragg diffraction and hard X-ray photoelectron spectroscopy (HAXPES) revealed a rock salt-like average structure with local distortions linked to cation coloring. Density functional theory (DFT) and crystal orbital Hamilton population (COHP) analyses confirmed that local Bi-rich and Ag-rich nanodomains amplify stereochemical activity, whereas more mixed and cation-order nanodomains are less stereochemically active. This local, nanoscopic mixing of segregated and ordered domains would indeed explain an average Fm3̅m structure that is rock salt-like and that does not manifest the full anharmonicity and noncentrosymmetry evidenced in canonical structures with stereochemical expression. These findings provide insights into the local structural and electronic complexities governing the optoelectronic properties of AgBiS 2 thin films.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Comparing plasma conditions in short-pulse-heated foils via fine-structure x-ray emission
Fine-structure x-ray spectra have been measured from foils with embedded tracer layers at two laser facilities. In this work, a suite of layered foils with thin Ti tracers under varied tamper layers was studied at both the Titan and the ALEPH 400 nm laser facilities, where Ti Heα emission was recorded using a high-resolution Bragg crystal spectrometer. Several indicators of plasma parameters are examined in the spectra, including temperature- and density-dependent line ratios and line broadening from Stark and opacity effects. Spectra indicate that (1) the plasma density at ALEPH is significantly higher than at Titan and (2) the electron temperature is high for near-surface layers at both facilities but drops more quickly with depth at ALEPH. These inferences of plasma conditions are consistent with differing levels of temporal contrast at each laser facility.
47 OTHER INSTRUMENTATION↗