Mending cracks atom-by-atom in rutile TiO2 with electron beam radiolysis

Guo, Silu; Yun, Hwanhui; Nair, Sreejith; Jalan, Bharat; Mkhoyan, K. Andre

doi:10.1038/s41467-023-41781-x

Mending cracks atom-by-atom in rutile TiO2 with electron beam radiolysis

Journal Article · Tue Sep 26 00:00:00 EDT 2023 · Nature Communications

DOI:https://doi.org/10.1038/s41467-023-41781-x· OSTI ID:2006548

; ; Nair, Sreejith; ;

Abstract

Rich electron-matter interactions fundamentally enable electron probe studies of materials such as scanning transmission electron microscopy (STEM). Inelastic interactions often result in structural modifications of the material, ultimately limiting the quality of electron probe measurements. However, atomistic mechanisms of inelastic-scattering-driven transformations are difficult to characterize. Here, we report direct visualization of radiolysis-driven restructuring of rutile TiO ₂ under electron beam irradiation. Using annular dark field imaging and electron energy-loss spectroscopy signals, STEM probes revealed the progressive filling of atomically sharp nanometer-wide cracks with striking atomic resolution detail. STEM probes of varying beam energy and precisely controlled electron dose were found to constructively restructure rutile TiO ₂ according to a quantified radiolytic mechanism. Based on direct experimental observation, a “two-step rolling” model of mobile octahedral building blocks enabling radiolysis-driven atomic migration is introduced. Such controlled electron beam-induced radiolytic restructuring can be used to engineer novel nanostructures atom-by-atom.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: NONE; SC0020211

OSTI ID:: 2006548

Alternate ID(s):: OSTI ID: 2421474

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 14; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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