arXiv subjects

Matthew Weyland

Publications and source records attributed to Matthew Weyland.

6 recordsLinked to original sources

arXiv2026

Structural properties of one-dimensional $\mathrm{Cs}_2\mathrm{CoCl}_4$ confined within single-walled carbon nanotubes

Crystals under one-dimensional (1D) confinement are well-known to exhibit drastic changes in metallicity, magnetic properties and chemical state, however, the intermediate phase space between binary metal halides and ternary metal halide perovskites remains poorly explored, especially in the context of the rich polymorphism exhibited by both families in the one-dimensional limit. Through aberration-corrected (scanning) transmission electron microscopy and multislice simulations, it is shown that the metal halide $\mathrm{Cs}_2\mathrm{CoCl}_4$ crystallizes in the tetragonal $\wp4/mcc$ and orthorhombic $\wp{mcm}$ rod groups under radial compression within single-walled carbon nanotubes (SWCNTs) of increasingly small diameter, with a massive re-entrant orthorhombic strain towards the $1$ $\mathrm{nm}$ extremum. The persistence of $\mathrm{Co}^{2+}$ is determined from fits to the d.c. magnetization, with a surprisingly small increase in the effective moment ($4.607(3)$ to $4.788(3) \mathit{{\mu}}_\mathrm{B}/\mathrm{f.u.}$) and Weiss constant ($-7.9(3)$ to $-4.09(7) \mathrm{K}$) after confinement in the SWCNTs, suggesting that the confined structure topologically preserves the core magnetic properties of the bulk. Both unconventional polymorphs observed are noticeably different to the high-pressure piezochromic polymorph previously shown to undergo a tetrahedral-to-octahedral coordination transition, highlighting 1D confinement as a unique tool for structural manipulation.

cond-mat.mtrl-sci↗

arXiv2025

Dopant site occupancy determined by core-loss-filtered, position-averaged convergent beam electron diffraction

In the elastic scattering regime, probe position-averaged convergent beam electron diffraction (PACBED) patterns have proven robust for estimating specimen thickness and mistilt. Through simulation, we show that core-loss-filtered PACBED patterns can be used to measure the site occupancy of a small concentration of dopants in an otherwise known crystal structure. By leveraging the reciprocity between scanning and conventional transmission electron microscopy, we interpret core-loss PACBED patterns using a strategy traditionally used for determining dopant concentrations via energy dispersive X-ray spectroscopy. We show that differences in the interaction range of different elements hinder a purely measurement-based quantification strategy, but that this can be overcome through comparison with simulations that generalize the Cliff-Lorimer k-factors.

cond-mat.other↗

arXiv2025

Quantitative structure determination from experimental four-dimensional scanning transmission electron microscopy via the scattering matrix

Considerable inroads have recently been made on algorithms to determine the sample potential from four-dimensional scanning transmission electron microscopy data from thick samples where multiple scattering cannot be neglected. This paper further develops the scattering matrix approach to such structure determination. Through simulation, we demonstrate how this approach can be modified to better handle partial spatial coherence, unknown probe defocus, and information from the dark field region. By combining these developments we reconstruct the electrostatic potential of a monolithic SrTiO$_3$ crystal showing good quantitative agreement with the expected structure.

cond-mat.mtrl-sci↗

arXiv2024

Differential phase contrast from electrons that cause inner shell ionization

Differential Phase Contrast (DPC) imaging, in which deviations in the bright field beam are in proportion to the electric field, has been extensively studied in the context of pure elastic scattering. Here we discuss differential phase contrast formed from core-loss scattered electrons, i.e. those that have caused inner shell ionization of atoms in the specimen, using a transition potential approach for which we study the number of final states needed for a converged calculation. In the phase object approximation, we show formally that differential phase contrast formed from core-loss scattered electrons is mainly a result of preservation of elastic contrast. Through simulation we demonstrate that whether the inelastic DPC images show element selective contrast depends on the spatial range of the ionization interaction, and specifically that when the energy loss is low the delocalisation can lead to contributions to the contrast from atoms other than that ionized. We further show that inelastic DPC images remain robustly interpretable to larger thicknesses than is the case for elastic DPC images, owing to the incoherence of the inelastic wavefields, though subtleties due to channelling remain. Lastly, we show that while a very high dose will be needed for sufficient counting statistics to discern differential phase contrast from core-loss scattered electrons, there is some enhancement of signal-to-noise ratio with thickness that makes inelastic DPC imaging more achievable for thicker samples.

cond-mat.other↗

arXiv2020

Tuning the convergence angle for optimum STEM performance

The achievable instrumental performance of a scanning transmission electron microscope (STEM) is determined by the size and shape of the incident electron probe. The most important optical factor in achieving the optimum probe profile is the radius of the probe-forming aperture, which determines the convergence semi-angle of the illumination. What is often overlooked however is that small deviations from this optimum can degrade both the resolution and interpretability of image contrast. A 30% error in aperture radius can lead to a factor of 2 contrast reduction in typical lattice spacings, and a 5 Å error in the thickness measurement of thin layers (such as gate oxides). Theoretical calculations of the optimum convergence angles, from a wave-optical consideration of the probe forming conditions, are explained and their consequences discussed. An experimental approach to the measurement and tuning of the convergence angle is then introduced. This is intended for uncorrected electron microscopes. For corrected instruments, Cs=0, and Cc usually determines the choice of aperture - see e.g. ULTRAMICROSCOPY 108, (2008) 1454-1466

cond-mat.mtrl-sci↗

arXiv2018

Structure retrieval at atomic resolution in the presence of multiple scattering of the electron probe

The projected electrostatic potential of a thick crystal is reconstructed at atomic-resolution from experimental scanning transmission electron microscopy data recorded using a new generation fast- readout electron camera. This practical and deterministic inversion of the equations encapsulating multiple scattering that were written down by Bethe in 1928 removes the restriction of established methods to ultrathin ($\lesssim 50$ Å) samples. Instruments already coming on-line can overcome the remaining resolution-limiting effects in this method due to finite probe-forming aperture size, spatial incoherence and residual lens aberrations.

cond-mat.mtrl-sci↗