Regensburg 2025 – wissenschaftliches Programm
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O: Fachverband Oberflächenphysik
O 42: Electron-driven Processes
O 42.4: Vortrag
Dienstag, 18. März 2025, 14:45–15:00, H11
Nonadiabatic quantum dynamics of molecules scattering from metal surfaces — •Riley Preston1, Yaling Ke2, Samuel Rudge1, Nils Hertl3, Raffaele Borrelli4, Reinhard Maurer3, and Michael Thoss1 — 1Institute of Physics, University of Freiburg — 2Department of Chemistry and Applied Biosciences, ETH Zürich — 3Department of Chemistry and Department of Physics, University of Warwick — 4DISAFA, University of Torino
Nonadiabatic coupling between electrons and molecular motion at metal surfaces can strongly impact the dynamics of a scattering molecule [1]. We present a theoretical approach based on hierarchical equations of motion (HEOM) [2], which models the scattering of molecules from metal surfaces and incorporates all nonadiabatic and quantum nuclear effects due to the coupling of the molecular degrees of freedom to the electrons in the metal. The approach is exemplified by its application to NO scattering from Au(111), where we observe multi-quantum relaxation of the bond vibrational state due to coupling to electron hole pairs in the surface, in accordance with experiment. The data obtained by the HEOM approach is also used as a rigorous benchmark to assess various mixed quantum-classical methods, from which we derive insights into the validity range of each method [3].
[1] A. M. Wodtke, Chem. Soc. Rev. 45, 3641-3657 (2016).
[2] Y. Ke, R. Borrelli, and M. Thoss, J. Chem. Phys. 156, 194102 (2022).
[3] R. J. Preston, Y. Ke, S. L. Rudge, N. Hertl, R. Borrelli, R. J. Maurer, and M. Thoss, arXiv preprint arXiv:2410.05142 (2024).
Keywords: Nonadiabatic dynamics; Molecule scattering; Quantum dynamics; Scattering from metal surfaces; Electron-hole pair