Quantum theory of electronic excitation and sputtering by transmission electron microscopy

Anthony Yoshimura; Michael Lamparski; Joel Giedt; David Lingerfelt; Jacek Jakowski; Panchapakesan Ganesh; Tao Yu; Bobby G. Sumpter; Vincent Meunier

doi:10.1039/D2NR01018F

Quantum theory of electronic excitation and sputtering by transmission electron microscopy†

Anthony Yoshimura,

*^ab Michael Lamparski,

^b Joel Giedt,

^b David Lingerfelt,

^c Jacek Jakowski,

^d Panchapakesan Ganesh,

^c Tao Yu,

‡^e Bobby G. Sumpter

^c and Vincent Meunier

^bf

Author affiliations

* Corresponding authors

^a Lawrence Livermore National Laboratory, Livermore, CA 94550, USA
E-mail: yoshimura4@llnl.gov

^b Department of Physics, Applied Physics, and Astronomy, Rensselaer Polytechnic Institute, Troy, NY 12180, USA

^c Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA

^d Computational Sciences and Engineering Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA

^e Department of Chemistry, University of North Dakota, Grand Forks, ND 58202, USA

^f Department of Materials Science and Engineering, Rensselaer Polytechnic Institute, Troy, NY 12180, USA

Abstract

Many computational models have been developed to predict the rates of atomic displacements in two-dimensional (2D) materials under electron beam irradiation. However, these models often drastically underestimate the displacement rates in 2D insulators, in which beam-induced electronic excitations can reduce the binding energies of the irradiated atoms. This bond softening leads to a qualitative disagreement between theory and experiment, in that substantial sputtering is experimentally observed at beam energies deemed far too small to drive atomic dislocation by many current models. To address these theoretical shortcomings, this paper develops a first-principles method to calculate the probability of beam-induced electronic excitations by coupling quantum electrodynamics (QED) scattering amplitudes to density functional theory (DFT) single-particle orbitals. The presented theory then explicitly considers the effect of these electronic excitations on the sputtering cross section. Applying this method to 2D hexagonal BN and MoS₂ significantly increases their calculated sputtering cross sections and correctly yields appreciable sputtering rates at beam energies previously predicted to leave the crystals intact. The proposed QED-DFT approach can be easily extended to describe a rich variety of beam-driven phenomena in any crystalline material.

This article is part of the themed collection: 2023 Nanoscale HOT Article Collection

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Quantum theory of electronic excitation and sputtering by transmission electron microscopy†

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