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Peter A. Crozier

Publications and source records attributed to Peter A. Crozier.

20 records · Page 2Linked to original sources

Tracking the Picoscale Spatial Motion of Atomic Columns During Dynamic Structural Change

In many materials systems, such as catalytic nanoparticles, the ability to characterize dynamic atomic structural changes is important for developing a more fundamental understanding of functionality. Recent developments in direct electron detection now allow image series to be acquired at frame rates on the order of 1000 frames per second in bright-field transmission electron microscopy (BF TEM), which could potentially allow dynamic changes in the atomic structure of individual nanoparticles to be characterized with millisecond temporal resolution in favourable cases. However, extracting such data from TEM image series requires the development of computational methods that can be applied to very large datasets and are robust in the presence of noise and in the non-ideal imaging conditions of some types of environmental TEM experiments. Here, we present a two-dimensional Gaussian fitting algorithm to track the position and intensities of atomic columns in temporally resolved BF TEM image series. We have tested our algorithm on experimental image series of Ce atomic columns near the surface of a ceria (CeO2) nanoparticle with electron beam doses of ~125-5000 e-Å-2 per frame. The accuracy of the algorithm for locating atomic column positions is compared to that of the more traditional centroid fitting technique, and the accuracy of intensity measurements is evaluated as a function of dose per frame. The code developed here, and the methodology used to explore the errors and limitations of the measurements, could be applied more broadly to any temporally resolved TEM image series to track dynamic atomic column motion.

cond-mat.mtrl-sci↗

Vibrational Spectroscopy at Atomic Resolution with Electron Impact Scattering

Atomic vibrations control all thermally activated processes in materials including diffusion, heat transport, phase transformations, and surface chemistry. Recent developments in monochromated, aberration-corrected scanning transmission electron microscopy (STEM) have enabled nanoscale probing of vibrational modes using a focused electron beam. However, to date, no experimental atomic resolution vibrational spectroscopy has been reported. Here we demonstrate atomic resolution by exploiting localized impact excitations of vibrational modes in materials. We show that the impact signal yields high spatial resolution in both covalent and ionic materials, and atomic resolution is available from both optical and acoustic vibrational modes. We achieve a spatial resolution of better than 2 Å which is an order of magnitude improvement compared to previous work. Our approach represents an important technical advance that can be used to provide new insights into the relationship between the thermal, elastic and kinetic properties of materials and atomic structural heterogeneities.

cond-mat.mtrl-sci↗