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O: Fachverband Oberflächenphysik
O 6: New Methods: Experiments and Theory
O 6.5: Vortrag
Montag, 27. März 2023, 11:30–11:45, GER 39
Surface-Sensitive Spectroscopy from First Principles — •Yair Litman1,2, Jinggang Lan3, Kuo-Yang Chiang2, Venkat Kapil1, Yuki Nagata2, and David Wilkins4 — 1University of Cambridge, Cambridge, United Kingdom — 2MPI for Polymer Research, Mainz, Germany — 3Ecole Polytechnique Fédérale de Lausanne, Lausanne, Switzerland — 4Queen’s University Belfast, Belfast, United Kingdom
Our current understanding of the structure and dynamics of aqueous interfaces at the molecular level has grown substantially in the last decades due to an increasing synergy between experimental measurements and atomistic simulations. However, the latter are either based on empirical force field models, which are neither suitable to describe bond breaking and formation nor systems with complex electronic structure, or on ab initio calculations which due to their computational cost cannot be statistically converged. In this work, we overcome all these limitations by combining high-dimensional neural network potentials with symmetry-adapted Gaussian process regression [1] to simulate the sum-frequency generation (SFG)[2] spectra of the water-air interface with ab initio accuracy. We obtain a good agreement with last-generation experiments and show how these models can in principle be improved systematically towards exact results. Overall, the machinery presented in this work paves the way for the modelling of surface-sensitive spectroscopy of complex interfaces. [1] V. Deringer, et al., Chem. Rev. 16, 121 (2021) [2] A. Morita, J. Hynes, J. Phys. Chem. B 106, 673 (2002).