Catalysis in Extreme Field Environments: A Case Study of Strongly Ionized SiO<sub>2</sub> Nanoparticle Surfaces

High electric fields can significantly alter catalytic environments and the resultant chemical processes. Such fields arise naturally in biological systems but can also be artificially induced through localized nanoscale excitations. Recently, strong field excitation of dielectric nanoparticles has emerged as an avenue for studying catalysis in highly ionized environments, producing extreme electric fields. While the dynamics of laser-driven surface ion emission has been extensively explored, understanding the molecular dynamics leading to fragmentation has remained elusive. Here, we employ a multiscale approach performing nonadiabatic quantum molecular dynamics (NAQMD) simulations on hydrogenated silica surfaces in both bare and wetted environments under field conditions mimicking those of an ionized nanoparticle. Our findings indicate that hole localization drives fragmentation dynamics, leading to surface silanol dissociation within 50 fs and charge transfer-induced water splitting in wetted environments within 150 fs. Further insight into such ultrafast mechanisms is critical for the advancement of catalysis on the surface of charged nanosystems.

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Publication Details

Journal
Journal of the American Chemical Society
Published
2024-09-27
DOI
https://doi.org/10.1021/jacs.4c08550
Citations
3
Primary Topic
Spectroscopy and Quantum Chemical Studies
Type
article
Field-Weighted Citation Impact
1.01

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article

Catalysis in Extreme Field Environments: A Case Study of Strongly Ionized SiO2 Nanoparticle Surfaces

Thomas Linker, Ken‐ichi Nomura, Priya D. Vashishta, Alexandra J. Feinberg et al.
3 citations
Journal of the American Chemical Society
Spectroscopy and Quantum Chemical Studies
1.01
article

Catalysis in Extreme Field Environments: A Case Study of Strongly Ionized SiO2 Nanoparticle Surfaces

Thomas Linker, Ken‐ichi Nomura, Priya D. Vashishta, Alexandra J. Feinberg, Fuyuki Shimojo, Uwe Bergmann, Adam M. Summers, Aiichiro Nakano, Matthias F. Kling, Samuel Sahel-Schackis, Ritika Dagar
article en
3 citations

Abstract

High electric fields can significantly alter catalytic environments and the resultant chemical processes. Such fields arise naturally in biological systems but can also be artificially induced through localized nanoscale excitations. Recently, strong field excitation of dielectric nanoparticles has emerged as an avenue for studying catalysis in highly ionized environments, producing extreme electric fields. While the dynamics of laser-driven surface ion emission has been extensively explored, understanding the molecular dynamics leading to fragmentation has remained elusive. Here, we employ a multiscale approach performing nonadiabatic quantum molecular dynamics (NAQMD) simulations on hydrogenated silica surfaces in both bare and wetted environments under field conditions mimicking those of an ionized nanoparticle. Our findings indicate that hole localization drives fragmentation dynamics, leading to surface silanol dissociation within 50 fs and charge transfer-induced water splitting in wetted environments within 150 fs. Further insight into such ultrafast mechanisms is critical for the advancement of catalysis on the surface of charged nanosystems.

Journal of the American Chemical SocietyVol. 146(40)
University of Southern California (US), University of Wisconsin–Madison (US), SLAC National Accelerator Laboratory (US), Ludwig-Maximilians-Universität München (DE), Kumamoto University (JP)
U.S. Department of Energy, Deutsche Forschungsgemeinschaft, Office of Science, Multidisciplinary University Research Initiative, Office of Naval Research, Basic Energy Sciences
Openalex Percentile: Top 24%
Spectroscopy and Quantum Chemical Studies
1.01
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