ArticleProceedings of the National Academy of Sciences of the United States of America2024
A theory of phonon-induced friction on molecular adsorbates.
Article in Proceedings of the National Academy of Sciences of the United States of America, 2024. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 2 papers.
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2 citing papers in PubMed.
- How Many Kelvins Are Equivalent to One Electron-Volt: An Investigation of Energy-Temperature Scaling in Catalysis.Precision chemistry · 2026Article
- A theory of phonon-induced friction on molecular adsorbates.Proceedings of the National Academy of Sciences of the United States of America · 2024Article
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2 authors.
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Abstract
In this manuscript, we provide a general theory for how surface phonons couple to molecular adsorbates. Our theory maps the extended dynamics of a surface's atomic vibrational motions to a generalized Langevin equation, and by doing so captures these dynamics in a single quantity: the non-Markovian friction. The different frequency components of this friction are the phonon modes of the surface slab weighted by their coupling to the adsorbate degrees of freedom. Using this formalism, we demonstrate that physisorbed species couple primarily to acoustic phonons while chemisorbed species couple to dispersionless local vibrations. We subsequently derive equations for phonon-adjusted reaction rates using transition state theory and demonstrate that these corrections improve agreement with experimental results for CO desorption rates from Pt(111).
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