arXiv subjects

Hugh Simons

Publications and source records attributed to Hugh Simons.

16 recordsLinked to original sources

arXiv2024

Heterogeneous antiferroelectric ordering in NaNbO3-SrSnO3 ceramics revealed by direct superstructure imaging

NaNbO3-based antiferroelectric materials offer a promising pathway towards greener and more cost-effective energy storage devices. However, their intrinsic structural instabilities often lead to reduced energy density that compromises their performance and longevity. In this brief communication, we demonstrate how Dark-Field X-ray Microscopy, when carried out on the characteristically weak 1/4{843}pc superstructure reflection, can map the antiferroelectric phase and its strain heterogeneity in typically small, deeply-embedded grains of a NaNbO3 and 0.95NaNbO3-0.05SrSnO3 ceramics, representative of different phase transition behavior. Our results clearly evidences the stabilizing effect of SrSnO3 on the antiferroelectric phase by enhancing the degree of mesostructural order. In doing so, our method establishes a new platform for exploring the impact of disorder on the long-range strain heterogeneity within antiferroelectrics and other materials with modulated crystal structures.

cond-mat.mtrl-sci↗

arXiv2024

X-ray induced grain boundary formation and grain rotation in Bi2Se3

Optimizing grain boundary characteristics in polycrystalline materials can improve their properties. Many processing methods have been developed for grain boundary manipulation, including the use of intense radiation in certain applications. In this work, we used X-ray free electron laser pulses to irradiate single-crystalline bismuth selenide (Bi2Se3) and observed grain boundary formation and subsequent grain rotation in response to the X-ray radiation. Our observations with simultaneous transmission X-ray microscopy and X-ray diffraction demonstrate how intense X- ray radiation can rapidly change size and texture of grains.

cond-mat.mtrl-sci↗

arXiv2024

Spatially resolved mapping of coherent twin relationships in DFXM measurements

With dark firld x-ray microscopy, it is possible to measure reciprocal space manps of localized volumes embedded deeply in a large sample. Ferroelastic materials contains elastic twins that display characteristing splitting of diffraction peaks. We show how to utilize established methods for analysing reciprocal space maps of elastically twinned materials to the analysis of dark-field x-ray microscopy data to detemin the exact kind of domain wall present in each probed volume, even when the domains are not spatially resolved.

cond-mat.mtrl-sci↗

arXiv2023

Imaging the Electric Field with X-Ray Diffraction Microscopy

The properties of semiconductors and functional dielectrics are defined by their response in electric fields, which may be perturbed by defects and the strain they generate. In this work, we demonstrate how diffraction-based X-ray microscopy techniques may be utilized to image the electric field in insulating crystalline materials. By analysing a prototypical ferro- and piezoelectric material, BaTiO$_{3}$, we identify trends that can guide experimental design towards imaging the electric field using any diffraction-based X-ray microscopy technique. We explain these trends in the context of dark-field X-ray microscopy, but the framework is also valid for Bragg scanning probe X-ray microscopy, Bragg coherent diffraction imaging and Bragg X-ray ptychography. The ability to quantify electric field distributions alongside the defects and strain already accessible via these techniques offers a more comprehensive picture of the often complex structure-property relationships that exist in many insulating and semiconducting materials.

cond-mat.mtrl-sci↗

arXiv2023

Electric-field-induced non-ergodic relaxor to ferroelectric transition in BiFeO3-xSrTiO3 ceramics

While BiFeO3-based solid solutions show great promise for applications in energy conversion and storage, realizing this promise necessitates understanding the structure-property relationship in particular pertaining to the relaxor-like characteristics often exhibited by solid solutions with polar-to-non-polar morphotropic phase boundaries. To this end, we investigated the role of the compositionally-driven relaxor state in (100-x)BiFeO3-xSrTiO3 [BFO-xSTO], via in situ synchrotron X-ray diffraction under bipolar electric-field cycling. The electric-field induced changes to the crystal structure, phase fraction and domain textures were monitored via the {111}pc, {200}pc, and 1/2{311}pc Bragg peaks. The dynamics of the intensities and positions of the (111) and (11-1) reflections reveal an initial non-ergodic regime followed by long-range ferroelectric ordering after extended poling cycles. The increased degree of random multi-site occupation in BFO-42STO compared to BFO-35STO is correlated with an increase of the critical electric field needed to induce the non-ergodic-to-ferroelectric transition, and a decrease in the degree of domain reorientation. Although both compositions show an irreversible transition to a long-range ferroelectric state, our results suggest that the weaker ferroelectric response in BFO-42STO is related to an increase in ergodicity. This, in turn, serves to guide the development of BFO-based systems into promising platform for further property engineering towards specific capacitor applications.

cond-mat.mtrl-sci↗

arXiv2022

Real-time imaging of acoustic waves in bulk materials with X-ray microscopy

Materials modelling and processing require experiments to visualize and quantify how external excitations drive the evolution of deep subsurface structure and defects that determine properties. Today, 3D movies with ~100-nm resolution of crystalline structure are regularly acquired in minutes to hours using X-ray diffraction based imaging. We present an X-ray microscope that improves this time resolution to <100 femtoseconds, with images attainable even from a single X-ray pulse. Using this, we resolve the propagation of 18-km/s acoustic waves in mm-sized diamond crystals, and demonstrate how mechanical energy thermalizes from picosecond to microsecond timescales. Our approach unlocks a vast range of new experiments of materials phenomena with intricate structural dynamics at ultrafast timescales.

cond-mat.mtrl-sci↗

arXiv2022

Simultaneous Bright- and Dark-Field X-ray Microscopy at X-ray Free Electron Lasers

The structures, strain fields, and defect distributions in solid materials underlie the mechanical and physical properties across numerous applications. Many modern microstructural microscopy tools characterize crystal grains, domains and defects required to map lattice distortions or deformation, but are limited to studies of the (near) surface. Generally speaking, such tools cannot probe the structural dynamics in a way that is representative of bulk behavior. Synchrotron X-ray diffraction based imaging has long mapped the deeply embedded structural elements, and with enhanced resolution, Dark Field X-ray Microscopy (DFXM) can now map those features with the requisite nm-resolution. However, these techniques still suffer from the required integration times due to limitations from the source and optics. This work extends DFXM to X-ray free electron lasers, showing how the $10^{12}$ photons per pulse available at these sources offer structural characterization down to 100 fs resolution (orders of magnitude faster than current synchrotron images). We introduce the XFEL DFXM setup with simultaneous bright field microscopy to probe density changes within the same volume. This work presents a comprehensive guide to the multi-modal ultrafast high-resolution X-ray microscope that we constructed and tested at two XFELs, and shows initial data demonstrating two timing strategies to study associated reversible or irreversible lattice dynamics.

cond-mat.mtrl-sci↗

arXiv2022

Unveiling the interaction mechanisms of electron and X-ray radiation with halide perovskite semiconductors using scanning nano-probe diffraction

The interaction of high-energy electrons and X-ray photons with soft semiconductors such as halide perovskites is essential for the characterisation and understanding of these optoelectronic materials. Using nano-probe diffraction techniques, which can investigate physical properties on the nanoscale, we perform studies of the interaction of electron and X-ray radiation with state-of-the-art (FA$_{0.79}$MA$_{0.16}$Cs$_{0.05}$)Pb(I$_{0.83}$Br$_{0.17}$)$_3$ hybrid halide perovskite films (FA, formamidinium; MA, methylammonium). We track the changes in the local crystal structure as a function of fluence using scanning electron diffraction and synchrotron nano X-ray diffraction techniques. We identify perovskite grains from which additional reflections, corresponding to PbBr$_2$, appear as a crystalline degradation phase after fluences of ~200 e$^-${\AA}$^{-2}$. These changes are concomitant with the formation of small PbI$_2$ crystallites at the adjacent high-angle grain boundaries, with the formation of pinholes, and with a phase transition from tetragonal to cubic. A similar degradation pathway is caused by photon irradiation in nano-X-ray diffraction, suggesting common underlying mechanisms. Our approach explores the radiation limits of these materials and provides a description of the degradation pathways on the nanoscale. Addressing high-angle grain boundaries will be critical for the further improvement of halide polycrystalline film stability, especially for applications vulnerable to high-energy radiation such as space photovoltaics.

cond-mat.mtrl-sci↗

arXiv2022

Simulating dark-field x-ray microscopy images with wave front propagation techniques

Dark-Field X-ray Microscopy (DFXM) is a diffraction-based synchrotron imaging techique capable of imaging defects in the bulk of extended crystalline samples. We present numerical simulations of image-formation in such a microscope using numerical integration of the dynamical Takagi-Taupin Equations (TTE) and wave front propagation. We validate our approach by comparing simulated images to experimental data from a near-perfect single crystal of diamond containing a single stacking fault defect in the illuminated volume.

cond-mat.mtrl-sci↗

arXiv2021

X-ray Free Electron Laser based Dark-Field X-ray Microscopy

Dark-field X-ray microscopy (DFXM) is a nondestructive full-field imaging technique providing three dimensional mapping of microstructure and local strain fields in deeply embedded crystalline elements. This is achieved by placing an objective lens in the diffracted beam, giving a magnified projection image. So far, the method has been applied with a time resolution of milliseconds to hours. In this work, we consider the feasibility of DFXM at the picosecond time scale using an X-ray free electron laser source and a pump-probe scheme. We combine thermomechanical strain wave simulations with geometrical optics and wavefront propagation optics to simulate DFXM images of phonon dynamics in a diamond single crystal. Using the specifications of the XCS instrument at the Linac Coherent Light Source (LCLS) as an example results in simulated DFXM images clearly showing the propagation of a strain wave.

cond-mat.mtrl-sci↗

arXiv2021

A finite difference scheme for integrating the Takagi-Taupin equations on an arbitrary orthogonal grid

Calculating dynamical diffraction patterns for X-ray topography and similar x-ray scattering-imaging techniques require the numerical integration of the Takagi-Taupin equations. This is usually performed with a simple second order finite difference scheme on a sheared computational grid with two of the axes aligned with the wave vectors of the incident and scattered beams respectively. This dictates, especially at low scattering angles, an oblique grid of uneven step-sizes. Here we present a finite difference scheme that carries out this integration in slab-shaped samples on an arbitrary orthogonal grid by implicitly utilizing Fourier interpolation. The scheme achieves the expected second order convergence and a similar error to the traditional approach on similarly dense grids.

physics.comp-ph↗

arXiv2020

Oxygen vacancies nucleate charged domain walls in ferroelectrics

We study the influence of oxygen vacancies on the formation of charged 180$^\circ$ domain walls in ferroelectric BaTiO$_3$ using first principles calculations. We show that it is favorable for vacancies to assemble in crystallographic planes, and that such clustering is accompanied by the formation of a charged domain wall. The domain wall has negative bound charge, which compensates the nominal positive charge of the vacancies and leads to a vanishing density of free charge at the wall. This is in contrast to the positively charged domain walls, which are nearly completely compensated by free charge from the bulk. The results thus explain the experimentally observed difference in electronic conductivity of the two types of domain walls, as well as the generic prevalence of charged domain walls in ferroelectrics. Moreover, the explicit demonstration of vacancy driven domain wall formation implies that specific charged domain wall configurations may be realized by bottom-up design for use in domain wall based information processing.

cond-mat.mes-hall↗

arXiv2020

In-Situ Visualization of Long-Range Defect Interactions at the Edge of Melting

Connecting a bulk material's microscopic defects to its macroscopic properties is an age-old problem in materials science. Long-range interactions between dislocations (line defects) are known to play a key role in how materials deform or melt, but we lack the tools to connect these dynamics to the macroscopic properties. We introduce time-resolved dark-field X-ray microscopy to directly visualize how dislocations move and interact over hundreds of micrometers, deep inside bulk aluminum. With real-time movies, we reveal the thermally-activated motion and interactions of dislocations that comprise a boundary, and show how weakened binding forces inhomogeneously destabilize the structure at 99% of the melting temperature. Connecting dynamics of the microstructure to its stability, we provide important opportunities to guide and validate multiscale models that are yet untested.

cond-mat.mtrl-sci↗

arXiv2019

Translative lens-based full field coherent X-ray imaging

We describe a full-field coherent imaging approach suitable for hard X-rays based on a classical (i.e. Galilean) X-ray microscope. The method combines a series of low-resolution images acquired at different transverse lens positions into a single high-resolution image, overcoming the spatial resolution limit set by the numerical aperture of the objective lens. We describe the optical principles of the approach, demonstrate the successful reconstruction of simulated phantom data, and discuss aspects of the reconstruction. We believe this approach offers some potential benefits over conventional scanning X-ray ptychography in terms of acquisition speed, spatial bandwidth and radiation dose rate.

physics.optics↗

arXiv2016

Extended formalism for simulating compound refractive lens-based x-ray microscopes

We present a comprehensive formalism for the simulation and optimisation of CRLs in both condensing and full-field imaging configurations. The approach extends ray transfer matrix analysis to account for x-ray attenuation by the lens material. Closed analytical expressions for critical imaging parameters such as numerical aperture, vignetting, chromatic aberration and focal length are provided for both thin- and thick-lens imaging geometries.

physics.optics↗

arXiv2015

Full-field hard x-ray microscopy with interdigitated silicon lenses

Full-field x-ray microscopy using x-ray objectives has become a mainstay of the biological and materials sciences. However, the inefficiency of existing objectives at x-ray energies above 15 keV has limited the technique to weakly absorbing or two-dimensional (2D) samples. Here, we show that significant gains in numerical aperture and spatial resolution may be possible at hard x-ray energies by using silicon-based optics comprising 'interdigitated' refractive silicon lenslets that alternate their focus between the horizontal and vertical directions. By capitalizing on the nano-manufacturing processes available to silicon, we show that it is possible to overcome the inherent inefficiencies of silicon-based optics and interdigitated geometries. As a proof-of-concept of Si-based interdigitated objectives, we demonstrate a prototype interdigitated lens with a resolution of ~255 nm at 17 keV.

physics.optics↗