Physics Discovery in Nanoplasmonic Systems via Autonomous Experiments in Scanning Transmission Electron Microscopy

Roccapriore, Kevin M.; Kalinin, Sergei V.; Ziatdinov, Maxim

doi:10.1002/advs.202203422

Physics Discovery in Nanoplasmonic Systems via Autonomous Experiments in Scanning Transmission Electron Microscopy

Journal Article · Sun Nov 06 23:00:00 EST 2022 · Advanced Science

DOI:https://doi.org/10.1002/advs.202203422· OSTI ID:1897253

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Center for Nanophase Materials Sciences Oak Ridge National Laboratory Oak Ridge TN 37831 USA
Center for Nanophase Materials Sciences Oak Ridge National Laboratory Oak Ridge TN 37831 USA, Department of Materials Science and Engineering University of Tennessee Knoxville TN 37916 USA
Center for Nanophase Materials Sciences Oak Ridge National Laboratory Oak Ridge TN 37831 USA, Computational Sciences and Engineering Division Oak Ridge National Laboratory Oak Ridge TN 37831 USA

Abstract

Physics‐driven discovery in an autonomous experiment has emerged as a dream application of machine learning in physical sciences. Here, this work develops and experimentally implements a deep kernel learning (DKL) workflow combining the correlative prediction of the target functional response and its uncertainty from the structure, and physics‐based selection of acquisition function, which autonomously guides the navigation of the image space. Compared to classical Bayesian optimization (BO) methods, this approach allows to capture the complex spatial features present in the images of realistic materials, and dynamically learn structure–property relationships. In combination with the flexible scalarizer function that allows to ascribe the degree of physical interest to predicted spectra, this enables physical discovery in automated experiment. Here, this approach is illustrated for nanoplasmonic studies of nanoparticles and experimentally implemented in a truly autonomous fashion for bulk‐ and edge plasmon discovery in MnPS ₃ , a lesser‐known beam‐sensitive layered 2D material. This approach is universal, can be directly used as‐is with any specimen, and is expected to be applicable to any probe‐based microscopic techniques including other STEM modalities, scanning probe microscopies, chemical, and optical imaging.

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Sponsoring Organization:: USDOE

OSTI ID:: 1897253

Alternate ID(s):: OSTI ID: 1897254
OSTI ID: 1901667

Journal Information:: Advanced Science, Journal Name: Advanced Science Journal Issue: 36 Vol. 9; ISSN 2198-3844

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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Physics Discovery in Nanoplasmonic Systems via Autonomous Experiments in Scanning Transmission Electron Microscopy

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Physics Discovery in Nanoplasmonic Systems via Autonomous Experiments in Scanning Transmission Electron Microscopy

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