Regensburg 2022 – wissenschaftliches Programm
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O: Fachverband Oberflächenphysik
O 46: New Methods and Developments 3: Theory
O 46.6: Vortrag
Mittwoch, 7. September 2022, 16:15–16:30, H6
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 Born-Oppenheimer approximation fails to capture the extent of multiquantum vibrational energy loss recorded during molecular scattering from metallic surfaces.[1] NO scattering on Au(111) has been one of the most studied examples in this regard, providing a testing ground for developing various nonadiabatic theories. The exact failings compared to experiment and their origin from theory are not established for any system, particularly since 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 the energy and the 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] C. L. Box & Y. Zhang et al, JACS Au, 2020 [2] R. Yin et al, J. Phys. Chem. Lett, 2019