SurfaceScience21 – wissenschaftliches Programm
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O: Fachverband Oberflächenphysik
O 63: Poster Session V: Electron-driven processes at surfaces and interfaces
O 63.1: Poster
Mittwoch, 3. März 2021, 10:30–12:30, P
Quantifying the breakdown of electronic friction theory during molecular scattering of NO from Au(111) — •Connor L. Box1, Yaolong Zhang2, Rongrong Yin2, Bin Jiang2, and Reinhard J. Maurer1 — 1Department of Chemistry, University of Warwick, United Kingdom — 2Department of Chemical Physics, University of Science and Technology of China, Hefei, China
The multiquantum vibrational energy loss recorded during molecular scattering from metallic surfaces is a testament to the breakdown of the Born-Oppenheimer approximation. Vibrational state-to-state scattering of NO on Au(111) has been one of the most studied examples in this regard, providing a testing ground for developing various nonadiabatic theories. However, the exact failings compared to experiment and their origin from theory are not established for any system because dynamic properties are affected by many compounding simulation errors of which the quality of nonadiabatic treatment is just one. We use a high dimensional machine learning representation of energy and electronic friction tensor to minimize errors that arise from quantum chemistry.[1,2] This allows us to perform a comprehensive quantitative analysis of the performance of molecular dynamics with electronic friction in describing state-to-state scattering. We find that electronic friction theory accurately predicts elastic and single-quantum energy loss, but underestimates multi-quantum energy loss and overestimates molecular trapping at high vibrational excitation. Our analysis reveals potential remedies to these issues. [1] R. Yin et al, J. Phys. Chem. Lett, 2019 [2] C. L. Box et al, JACS Au, 2020