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83 records · Page 5

Antiferromagnetic real-space configuration probed by dichroism in scattered x-ray beams with orbital angular momentum

X-ray beams with orbital angular momentum (OAM) are a promising tool for x-ray characterization techniques. Beams with OAM have a helicity - an azimuthally varying phase - which leads to a gradient of the light field. New material properties can be probed by utilizing the helicity of an OAM beam. Here, we demonstrate a dichroic effect in resonant diffraction from an artificial antiferromagnet with a topological defect. We found that the scattered OAM beam has circular dichroism at the antiferromagnetic Bragg peak whose sign is coupled to its helicity, which reveals the real-space configuration of the antiferromagnetic ground state. Thermal cycling of the artificial antiferromagnet can change the ground state, as indicated by reversal of the sign of circular dichroism. This result is one of the first demonstrations of a soft x-ray spectroscopy characterization technique utilizing the OAM of x rays. In conclusion, this helicity-dependent circular dichroism exemplifies the potential to utilize OAM beams to probe matter in a way that is inaccessible using currently available x-ray techniques.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Atomically Resolved Acoustic Dynamics Coupled with Magnetic Order in a Van der Waals Antiferromagnet

Magnetoelastic coupling in van der Waals (vdW) magnetic materials enables a unique interplay between the spin and lattice degrees of freedom. Characterizing the elastic responses with atomic and femtosecond resolution across the magnetic transition is essential for guiding the design of magnetically tunable actuators and strain-mediated spintronic devices. Here, ultrafast X-ray diffraction employed at a free-electron laser reveals that the atomic displacements, wave vectors, and dispersion relations of acoustic phonon modes in a vdW antiferromagnet FePS3 are coupled with the magnetic order, by tracking both in-plane and out-of-plane Bragg peaks upon optical excitation across the Néel temperature (TN). One transverse mode shows that a quasi-out-of-plane atomic displacement undergoes a significant directional change across TN. Its quasi-in-plane wave vector is derived by comparing the measured sound velocity and the first-principles calculations. The other transverse mode is an interlayer shear acoustic mode whose amplitude is strongly enhanced in the antiferromagnetic phase, exhibiting eight times stronger amplitude than the longitudinal acoustic mode below TN. The atomically resolved characterization of acoustic phonon dynamics that couple with magnetic ordering opens opportunities for harnessing unique magnetoelastic coupling in vdW magnets on ultrafast timescales.

coherent acoustic phonons↗

X-ray optics for the cavity-based X-ray free-electron laser

A cavity-based X-ray free-electron laser (CBXFEL) is a possible future direction in the development of fully coherent X-ray sources. CBXFELs consist of a low-emittance electron source, a magnet system with several undulators and chicanes, and an X-ray cavity. The X-ray cavity stores and circulates X-ray pulses for repeated FEL interactions with electron pulses until the FEL reaches saturation. CBXFEL cavities require low-loss wavefront-preserving optical components: near-100%-reflectivity X-ray diamond Bragg-reflecting crystals, outcoupling devices such as thin diamond membranes or X-ray gratings, and aberration-free focusing elements. In the framework of the collaborative CBXFEL research and development project of Argonne National Laboratory, SLAC National Accelerator Laboratory and SPring-8, we report here the design, manufacturing and characterization of X-ray optical components for the CBXFEL cavity, which include high-reflectivity diamond crystal mirrors, a diamond drumhead crystal with thin membranes, beryllium refractive lenses and channel-cut Si monochromators. All the designed optical components have been fully characterized at the Advanced Photon Source to demonstrate their suitability for the CBXFEL cavity application.

47 OTHER INSTRUMENTATION↗

Operando Bragg Coherent Diffraction Imaging of LiNi 0.8 Mn 0.1 Co 0.1 O 2 Primary Particles within Commercially Printed NMC811 Electrode Sheets

Due to complex degradation mechanisms, disparities between the theoretical and practical capacities of lithium-ion battery cathode materials persist. Specifically, Ni-rich chemistries such as LiNi 0.8 Mn 0.1 Co 0.1 O 2 (or NMC811) are one of the most promising choices for automotive applications; however, they continue to suffer severe degradation during operation that is poorly understood, thus challenging to mitigate. Here in this paper we use operando Bragg coherent diffraction imaging for 4D analysis of these mechanisms by inspecting the individual crystals within primary particles at various states of charge (SoC). Although some crystals were relatively homogeneous, we consistently observed non-uniform distributions of inter- and intracrystal strain at all measured SoC. Pristine structures may already possess heterogeneities capable of triggering crystal splitting and subsequently particle cracking. During low-voltage charging (2.7–3.5 V), crystal splitting may still occur even during minimal bulk deintercalation activity; and during discharging, rotational effects within parallel domains appear to be the precursor for the nucleation of screw dislocations at the crystal core. Ultimately, this discovery of the central role of crystal grain splitting in the charge/discharge dynamics may have ramifications across length scales that affect macroscopic performance loss during real-world battery operation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Electric field driven domain wall dynamics in BaTiO 3 nanoparticles

We report a detailed investigation into the response of single BaTiO 3 (BTO) nanocrystals under applied electric fields (E-field) using Bragg coherent diffraction imaging. Our study reveals pronounced domain wall migration and expansion of a sample measure under applied electric field. The changes are most prominent at the surface of the nanocrystal, where the lack of external strain allows greater domain wall mobility. The observed domain shifts are correlated to the strength and orientation of the applied E-field, following a side-by-side domain model from Suzana []. Notably, we identified a critical electric field strength of 3 MV/m, which leads to irreversible structural changes, suggesting plastic deformation. The findings highlight how surface effects and intrinsic defects contribute to the enhanced dielectric properties of BTO at the nanoscale, in contrast to bulk materials, where strain limits domain mobility. These findings deepen our understanding of nanoscale dielectric behavior and inform the design of advanced nanoelectronic devices. Published by the American Physical Society 2025

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Probing Fundamental Mechanisms of Plastic Deformation with High Energy X-rays (Final Progress Report)

Overall, substantial progress was made on developing BCDI techniques in the direction of imaging defects in multi-crystal samples. Section 2.1 describes a new method to reconstruct the 3D atomic displacement field within a grain from multiple coherently resolved diffraction peaks. The key development is the ability to recover a best fit to the grain shape at the same time as the internal displacement (strain) variation with no prior knowledge of the microstructure. This is complemented by the development of a method, Sec. 2.2, to separate out sets of Laue reflections that belong to a single grain (and thus be able to index its orientation) in the commonly encountered situation in which the beam illuminates several grains in a given location. This is essential for enabling collection of coherent diffraction data (at APS 34-ID-C) from neighboring grains. All experiments depend on the quality of samples used. Although good progress has been made with thin film samples, we are working with a broader range of geometries. A new sample design uses a high-Z metal (e.g., Pt) deposited in a sub-micron trench in a low-Z metal (e.g., Al) so that the grain size is prevented from exceeding the current limit for BCDI. We also report in section 3.1 on successfully applying NF-HEDM to a fine-grain Mg sample that would normally be considered out of scope for the method. This represents progress towards being able to map out polycrystalline samples in 3D before performing BCDI on individual grains. We further report in section 3.2 on preliminary NF-HEDM characterization of a sample of UO2 that has sub-micron grains; the data imply the capability of mapping fine-grain polycrystals at 1-ID-E, again for the purposes of BCDI in the bulk. Lastly, our plan is to load grains in polycrystalline samples by inducing thermal stress. We also report the experimental measurements of the Ti- 6Al-4V alloy obtained at the European Synchrotron Radiation Facility (ESRF), which had been indexed and mapped via HEDM at APS in section 9. As discussed below, however, technique development pre-occupied the team throughout the project which meant that we did not make any significant progress towards answering the original hypotheses as stated in the proposal. In summary, we assert that we have made good progress in methods and samples and future work taking advantage of this progress is likely to obtain and analyze BCDI data from multiple adjacent grains in 3D polycrystals. Obtaining such data depends on re-gaining access to the Advanced Photon Source, which is anticipated in late summer or the Fall. In all cases, work has involved close collaboration with faculty, staff, postdocs and students from Brigham Young University (BYU), the Los Alamos National Laboratory and APS beamlines 1-ID and 34-ID.

36 MATERIALS SCIENCE↗

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

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

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Mechanistic Insights into Defect-Mediated Crystallization Revealed by Lattice Strain Evolution

Structural defects and lattice strain are intrinsic to many crystalline materials, yet their roles in controlling chemical reaction mechanisms and directing crystallization pathways remain poorly understood. Here, in this study, we revealed the three-dimensional evolution of strain and dislocation defects at the nanoscale during the growth of heterogeneously nucleated barite (BaSO 4 ) and calcite (CaCO 3 ) crystals by using coherent X-ray scattering, electron microscopy, and molecular simulations. Unlike barite, which formed with minimal internal strain, calcite developed dislocation defects and exhibited spatially varying strain that increased during growth. During growth in Sr-rich solutions, calcite likely incorporates Sr 2+ into the defects, which further modulates the local lattice structure and increases both the compressive and tensile strain. These findings suggest that calcite crystallization was likely dominated by attachment of precursor phases, which gave rise to defect-enriched domain structures not predicted by classical growth models. By linking defect formation to ion incorporation and growth dynamics, this work provides fundamental insight into how lattice-level strain heterogeneity governs the chemical reactivity of ionic crystals.

Bragg coherent diffractive imaging↗

X-ray Nanoimaging of Crystal Defects in Single Grains of Solid-State Electrolyte Li 7–3x Al x La 3 Zr 2 O 12

All-solid-state lithium batteries promise significant improvements in energy density and safety over traditional liquid electrolyte batteries. The Al-doped Li 7 La 3 Zr 2 O 12 (LLZO) solid-state electrolyte shows excellent potential given its high ionic conductivity and good thermal, chemical, and electrochemical stability. Nevertheless, further improvements on electrochemical and mechanical properties of LLZO call for an in-depth understanding of its local microstructure. Here, we employ Bragg coherent diffractive imaging to investigate the atomic displacements inside single grains of LLZO with various Al-doping concentrations, resulting in cubic, tetragonal, and cubic-tetragonal mixed structures. We observe coexisting domains of different crystallographic orientations in the tetragonal structure. We further show that Al doping leads to crystal defects such as dislocations and phase boundaries in the mixed- and cubic-phase grain. This study addresses the effect of Al doping on the nanoscale structure within individual grains of LLZO, which is informative for the future development of solid-state batteries.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Ultrafast Bragg coherent diffraction imaging of epitaxial thin films using deep complex-valued neural networks

Abstract Domain wall structures form spontaneously due to epitaxial misfit during thin film growth. Imaging the dynamics of domains and domain walls at ultrafast timescales can provide fundamental clues to features that impact electrical transport in electronic devices. Recently, deep learning based methods showed promising phase retrieval (PR) performance, allowing intensity-only measurements to be transformed into snapshot real space images. While the Fourier imaging model involves complex-valued quantities, most existing deep learning based methods solve the PR problem with real-valued based models, where the connection between amplitude and phase is ignored. To this end, we involve complex numbers operation in the neural network to preserve the amplitude and phase connection. Therefore, we employ the complex-valued neural network for solving the PR problem and evaluate it on Bragg coherent diffraction data streams collected from an epitaxial La 2-x Sr x CuO 4 (LSCO) thin film using an X-ray Free Electron Laser (XFEL). Our proposed complex-valued neural network based approach outperforms the traditional real-valued neural network methods in both supervised and unsupervised learning manner. Phase domains are also observed from the LSCO thin film at an ultrafast timescale using the complex-valued neural network.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Static and dynamic topological defects in the domain textures in the helical antiferromagnet Ni 2 ⁢CoTeO 6

Real-space Bragg coherent x-ray-diffractive imaging unveils the formation of bubble and stripe antiferromagnetic (AFM) phase domains on the surface of Ni 2 ⁢CoTeO 6 single crystal. The stripe domains exhibit dislocation-type topological defects. The defects typically form as defect-antidefect pairs and can be created or annihilated by temperature changes and local heating. Thermal fluctuations of the AFM domain walls are observed near the Néel temperature. Topological defect pairs dynamically form and disappear in the fluctuating state. These observations provide a real-space perspective on the dynamics of the AFM phase transition in a helical antiferromagnet. Finally, the remarkable tunability of AFM domain walls in a helical antiferromagnet underscores their potential for AFM spintronics applications.

36 MATERIALS SCIENCE↗