Controlling radiolysis chemistry on the nanoscale in liquid cell scanning transmission electron microscopy

文献情報

出版日 2021-03-09

DOI 10.1039/D0CP06369J

インパクトファクター 3.676

著者

Juhan Lee, Daniel Nicholls, B. Layla Mehdi

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要旨

When high-energy electrons from a scanning transmission electron microscope (STEM) are incident on a liquid, the vast majority of the chemical reactions that are observed are induced by the radiolysis breakdown of the liquid molecules. In the study of liquids, the radiolysis products of pure water are well known, and their rate of formation for a given flux of high-energy electrons has been studied intensively over the last few years for uniform TEM illumination. In this paper, we demonstrate that the temporal and spatial distribution of the electron illumination can significantly affect the final density of radiolysis products in water and even change the type of reaction taking place. We simulate the complex array of possible spatial/temporal distributions of electrons that are accessible experimentally by controlling the size, the scan rate and the hopping distance of the electron probe in STEM mode and then compare the results to the uniformly illuminated TEM mode of imaging. By distributing the electron dose both spatially and temporally in the STEM through a randomised “spot-scan” mode of imaging, the diffusion overlap of the radiolysis products can be reduced, and the resulting reactions can be more readily controlled. This control allows the resolution of the images to be separated from the speed of the induced reaction (which is based on beam current alone) and this facet of the experiment will allow a wide range of chemical reactions to be uniquely tailored and observed in all liquid cell STEM experiments.

掲載誌

Physical Chemistry Chemical Physics

CiteScore: 5.5

自己引用率: 10.3%

年間論文数: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.