arXiv subjects

Ross Harder

Publications and source records attributed to Ross Harder.

15 recordsLinked to original sources

arXiv2025

Spatio-temporal migration of antiferromagnetic domain walls in Sr2IrO4

By laser pump-probe time-resolved coherent magnetic X-ray diffraction imaging, we have measured the migration velocity of antiferromagnetic domain walls in the Mott insulator Sr2IrO4 at 100 K. During the laser-induced demagnetization, we observe domain walls moving at 3x10^6 m/s, significantly faster than acoustic velocities. This is understood to arise from a purely electronic spin contribution to the magnetic structure without any role for coupling to the crystal lattice.

cond-mat.str-el↗

arXiv2024

Manipulating ferroelectric topological polar structures with twisted light

The dynamic control of novel states of matter beyond thermodynamic equilibrium is a fundamental pursuit in condensed matter physics. Intense terahertz fields have enabled metal-insulator transitions, superconductivity, quantum paraelectric ferroelectricity, and room-temperature magnetization via circularly polarized terahertz electric fields. These effects hinge on the excitation of infrared-active soft phonon modes by terahertz fields. Expanding this concept, recent theory suggests that ferroelectric polarization may be manipulated through terahertz twisted light, transferring orbital angular momentum to create ferroelectric skyrmions. Our study experimentally demonstrates that such control is possible in quasi-2D ferroelectric CsBiNb2O7 using twisted UV light with orbital angular momentum (OAM). By resonantly exciting both the ferroelectric mode and the octahedral tilting mode, twisted UV light dynamically modulates the ferroelectric polarization. We employ in-situ X-ray Bragg coherent diffractive imaging, twisted optical Raman spectroscopy, and density functional theory to three-dimensionally resolve ionic displacement fields and polarization texture changes. Our observations reveal deterministic, reversible twisted light-induced strain and ionic displacements within the unit cell, causing substantial microscopic polarization changes. This interaction between twisted photons, phonon modes, and induced ionic displacements breaks symmetry and stabilizes a non-equilibrium ferroelectric phase with topological solitons. These findings offer a new path to control ferroelectricity and magnetism, opening avenues for novel optoelectronic devices such as ultrafast non-volatile memory switches by using light to coherently control ferroic states.

cond-mat.mtrl-sci↗

arXiv2023

Operando real-space imaging of a structural phase transformation in a high-voltage electrode

Discontinuous solid-solid phase transformations play a pivotal role in determining properties of rechargeable battery electrodes. By leveraging operando Bragg Coherent Diffractive Imaging (BCDI), we investigate the discontinuous phase transformation in LixNi0.5Mn1.5O4 within a fully operational battery. Throughout Li-intercalation, we directly observe the nucleation and growth of the Li-rich phase within the initially charged Li-poor phase in a 500 nm particle. Supported by the microelasticity model, the operando imaging unveils an evolution from a curved coherent to planar semi-coherent interface driven by dislocation dynamics. We hypothesize these dislocations exhibit a glissile motion that facilitates interface migration without diffusion of host ions, leaving the particle defect-free post-transformation. Our data indicates negligible kinetic limitations impacting the transformation kinetics, even at discharge rates as fast as C/2. This study underscores BCDI's capability to provide operando insights into nanoscale phase transformations, offering valuable guidance for electrochemical materials design and optimization.

cond-mat.mtrl-sci↗

arXiv2023

Manipulating Metastability: Quenched Control of Topological Defects in Multiferroics

The topological properties of quasiparticles, such as skyrmions and vortices, have the potential to offer extraordinary metastability through topological protection, and drive motion with minimal electrical current excitation. This has promising implications for future applications in spintronics. Skyrmions frequently appear either in lattice form or as separate, isolated quasiparticles \cite{Tokura21}. Magnetic ferroelectrics, a subset of multiferroics that exhibit magnetically induced ferroelectricity, possess intriguing characteristics like magnetic (electric) field-controlled ferroelectric (magnetic) responses. Previous research based on Landau theory indicated the potential to stabilize metastable phases in multiferroic barium hexaferrite \cite{Karpov19}. We have successfully stabilized these meta-stable phases through magnetic quenching of hexaferrite nanoparticles, leading to the creation of compelling topological structures. The structural changes in individual BaFe$_{12}$O$_{19}$ nanocrystals were scrutinized using Bragg coherent diffractive imaging, granting us insight into the emergent topological structures in field-quenched multiferroics. Additionally, we explored why these structures are energetically preferable for the formation of metastable topological structures.

cond-mat.mtrl-sci↗

arXiv2023

Enhanced piezoelectric response at nanoscale vortex structures in ferroelectrics

The piezoelectric response is a measure of the sensitivity of a material's polarization to stress or its strain to an applied field. Using in-operando x-ray Bragg coherent diffraction imaging, we observe that topological vortices are the source of a five-fold enhancement of the piezoelectric response near the vortex core. The vortices form where several low symmetry ferroelectric phases and phase boundaries coalesce. Unlike bulk ferroelectric solid solutions in which a large piezoelectric response is associated with coexisting phases in the proximity of the triple point, the largest responses for pure BaTiO3 at the nanoscale are in spatial regions of extremely small spontaneous polarization at vortex cores. The response decays inversely with polarization away from the vortex, analogous to the behavior in bulk ceramics as the cation compositions are varied away from the triple point. We use first-principles-based molecular dynamics to augment our observations, and our results suggest that nanoscale piezoelectric materials with large piezoelectric response can be designed within a parameter space governed by vortex cores. Our findings have implications for the development of next-generation nanoscale piezoelectric materials.

cond-mat.mtrl-sci↗

arXiv2022

Strain and Crystallographic Identification of the Helically Concaved Surfaces of Nanoparticles

Identifying the three-dimensional (3D) crystal-plane and strain-field distributions of nanocrystals is essential for optical, catalytic, and electronic applications. Here, we developed a methodology for visualizing the 3D information of chiral gold nanoparticles with concave gap structures by Bragg coherent X-ray diffraction imaging. The distribution of the high-Miller-index planes constituting the concave chiral gap was precisely determined. The highly strained region adjacent to the chiral gaps was resolved, which was correlated to the 432-symmetric morphology of the nanoparticles and its corresponding plasmonic properties were numerically predicted from the atomically defined structures. This approach can serve as a general characterization platform for visualizing the 3D crystallographic and strain distributions of nanoparticles, especially for applications where structural complexity and local heterogeneity are major determinants, as exemplified in plasmonics.

cond-mat.mtrl-sci↗

arXiv2021

Disorder Dynamics in Battery Nanoparticles During Phase Transitions Revealed by Operando Single-Particle Diffraction

Structural and ion-ordering phase transitions limit the viability of sodium-ion intercalation materials in grid scale battery storage by reducing their lifetime. However, the combination of phenomena in nanoparticulate electrodes creates complex behavior that is difficult to investigate, especially on the single nanoparticle scale under operating conditions. In this work, operando single-particle x-ray diffraction (oSP-XRD) is used to observe single-particle rotation, interlayer spacing, and layer misorientation in a functional sodium-ion battery. oSP-XRD is applied to Na$_{2/3}$[Ni$_{1/3}$Mn$_{2/3}$]O$_{2}$, an archetypal P2-type sodium-ion positive electrode material with the notorious P2-O2 phase transition induced by sodium (de)intercalation. It is found that during sodium extraction, the misorientation of crystalline layers inside individual particles increases before the layers suddenly align just prior to the P2-O2 transition. The increase in the long-range order coincides with an additional voltage plateau signifying a phase transition prior to the P2-O2 transition. To explain the layer alignment, a model for the phase evolution is proposed that includes a transition from localized to correlated Jahn-Teller distortions. The model is anticipated to guide further characterization and engineering of sodium-ion intercalation materials with P2-O2 type transitions. oSP-XRD therefore opens a powerful avenue for revealing complex phase behavior in heterogeneous nanoparticulate systems.

cond-mat.mtrl-sci↗

arXiv2020

Combining Laue diffraction with Bragg coherent diffraction imaging at 34-ID-C

Measurement modalities in Bragg coherent diffraction imaging (BCDI) rely on finding signal from a single nanoscale crystal object, which satisfies the Bragg condition among a large number of arbitrarily oriented nanocrystals. However, even when the signal from a single Bragg reflection with (hkl) Miller indices is found, the crystallographic axes on the retrieved three-dimensional (3D) image of the crystal remain unknown, and thus, localizing in reciprocal space other Bragg reflections becomes in reality impossible or requires good knowledge of the orientation of the crystal. We report the commissioning of a movable double-bounce Si (111) monochromator at the 34-ID-C end station of the Advanced Photon Source, which aims at delivering multi-reflection BCDI as a standard tool in a single beamline instrument. The new instrument enables this through rapid switching from monochromatic to broadband (pink) beam permitting the use of Laue diffraction to determine crystal orientation. With a proper orientation matrix determined for the lattice, one can measure coherent diffraction near multiple Bragg peaks, thus providing sufficient information to image the full strain tensor in 3D. We discuss the design, concept of operation, the developed procedures for indexing Laue patterns, and automated measuring of Bragg coherent diffraction data from multiple reflections of the same nanocrystal.

physics.ins-det↗

arXiv2019

Gas-induced segregation in Pt-Rh alloy nanoparticles observed by in-situ Bragg coherent diffraction imaging

Bimetallic catalysts can undergo segregation or redistribution of the metals driven by oxidizing and reducing environments. Bragg coherent diffraction imaging (BCDI) was used to relate displacement fields to compositional distributions in crystalline Pt-Rh alloy nanoparticles. 3D images of internal composition showed that the radial distribution of compositions reverses partially between the surface shell and the core when gas flow changes between O2 and H2. Our observation suggests that the elemental segregation of nanoparticle catalysts should be highly active during heterogeneous catalysis and can be a controlling factor in synthesis of electrocatalysts. In addition, our study exemplifies applications of BCDI for in situ 3D imaging of internal equilibrium compositions in other bimetallic alloy nanoparticles.

cond-mat.mtrl-sci↗

arXiv2019

High-energy coherent X-ray diffraction microscopy of polycrystal grains: first steps towards a multi-scale approach

We present proof-of-concept imaging measurements of a polycrystalline material that integrate the elements of conventional high-energy X-ray diffraction microscopy with coherent diffraction imaging techniques, and that can enable in-situ strain-sensitive imaging of lattice structure in ensembles of deeply embedded crystals over five decades of length scale upon full realization. Such multi-scale imaging capabilities are critical to addressing important questions in a variety of research areas such as materials science and engineering, chemistry, and solid state physics. Towards this eventual goal, the following key aspects are demonstrated: 1) high-energy Bragg coherent diffraction imaging (HE-BCDI) of sub-micron-scale crystallites at 52 keV at current third-generation synchrotron light sources, 2) HE-BCDI performed in conjunction with far-field high-energy diffraction microscopy (ff-HEDM) on the grains of a polycrystalline sample in an smoothly integrated manner, and 3) the orientation information of an ensemble of grains obtained via ff-HEDM used to perform complementary HE-BCDI on multiple Bragg reflections of a single targeted grain. These steps lay the foundation for integration of HE-BCDI, which typically provides a spatial resolution tens of nanometers, into a broad suite of well-established HEDM methods, extending HEDM beyond the few-micrometer resolution bound and into the nanoscale, and positioning the approach to take full advantage of the orders-of-magnitude improvement of X-ray coherence expected at fourth generation light sources presently being built and commissioned worldwide.

cond-mat.mtrl-sci↗

arXiv2018

Phase retrieval for Bragg coherent diffraction imaging at high X-ray energies

Coherent X-ray beams with energies $\geq 50$ keV can potentially enable three-dimensional imaging of atomic lattice distortion fields within individual crystallites in bulk polycrystalline materials through Bragg coherent diffraction imaging (BCDI). However, the undersampling of the diffraction signal due to Fourier space compression at high X-ray energies renders conventional phase retrieval algorithms unsuitable for three-dimensional reconstruction. To address this problem we utilize a phase retrieval method with a Fourier constraint specifically tailored for undersampled diffraction data measured with coarse-pitched detector pixels that bin the underlying signal. With our approach, we show that it is possible to reconstruct three-dimensional strained crystallites from an undersampled Bragg diffraction data set subject to pixel-area integration without having to physically upsample the diffraction signal. Using simulations and experimental results, we demonstrate that explicit modeling of Fourier space compression during phase retrieval provides a viable means by which to invert high-energy BCDI data, which is otherwise intractable.

cond-mat.mtrl-sci↗

arXiv2017

Sparse recovery of undersampled intensity patterns for coherent diffraction imaging at high X-ray energies

Coherent X-ray photons with energies higher than 50 keV offer new possibilities for imaging nanoscale lattice distortions in bulk crystalline materials using Bragg peak phase retrieval methods. However, the compression of reciprocal space at high energies typically results in poorly resolved fringes on an area detector, rendering the diffraction data unsuitable for the three-dimensional reconstruction of compact crystals. To address this problem, we propose a method by which to recover fine fringe detail in the scattered intensity. This recovery is achieved in two steps: multiple undersampled measurements are made by in-plane sub-pixel motion of the area detector, then this data set is passed to a sparsity-based numerical solver that recovers fringe detail suitable for standard Bragg coherent diffraction imaging (BCDI) reconstruction methods of compact single crystals. The key insight of this paper is that sparsity in a BCDI data set can be enforced by recognising that the signal in the detector, though poorly resolved, is band-limited. This requires fewer in-plane detector translations for complete signal recovery, while adhering to information theory limits. We use simulated BCDI data sets to demonstrate the approach, outline our sparse recovery strategy, and comment on future opportunities.

eess.SP↗

arXiv2017

Bragg projection ptychography on niobium phase domain

We demonstrate that the highly sensitive phase-contrast properties of Bragg coherent diffraction measurements combined with the translational diversity of ptychography can provide a Bragg "dark field" imaging method capable of revealing the finger print of domain structure in metallic thin films. Experimental diffraction data was taken from a epitaxially grown niobium metallic thin film on sapphire; and analysed with the help of a careful combination of implemented refinement mechanisms.

cond-mat.mtrl-sci↗

arXiv2016

In-situ 3D Imaging of Catalysis Induced Strain in Gold Nanoparticles

Multi-electron transfer processes, such as hydrogen and oxygen evolution reactions, are crucially important in energy and biological science but require favorable catalysts to achieve fast kinetics. Nanostructuring catalysts can dramatically improve their properties, which can be difficult to understand due to strain and size dependent thermodynamics, the influence of defects, and substrate dependent activities. Here, we report 3D imaging of single gold nanoparticles during catalysis of ascorbic acid decomposition using Bragg coherent diffractive imaging (BCDI) as a route to eliminate ensemble effects while elucidating the strain-activity connection. Local strains were measured in single nanoparticles and modeled using reactive molecular dynamics (RMD) simulations and finite element analysis (FEA) simulations. RMD reveals a new chemical pathway for local strain generation in the gold lattice: chemisorption of hydroxyl ions. FEA reveals that the RMD results are transferable to the larger nanocrystal sizes studied in the experiment. Our study reveals the strain-activity connection and opens a powerful new avenue for joint theoretical and experimental studies of multi-electron transfer processes catalyzed by nanocrystals.

cond-mat.mtrl-sci↗

arXiv2012

Probing the three-dimensional strain inhomogeneity and equilibrium elastic properties of single crystal Ni nanowires

We employ three dimensional x-ray coherent diffraction imaging to map the lattice strain distribution, and to probe the elastic properties of a single crystalline Ni (001) nanowire grown vertically on an amorphous Si02 || Si substrate. The reconstructed density maps show that with increasing wire width, the equilibrium compressive stress in the core region decreases sharply while the surface tensile strain increases, and gradually trends to a nonzero constant. We use the retrieved projection of lattice distortion to predict the Young's Modulus of the wire based on the elasticity theory.

cond-mat.mes-hall↗