Regensburg 2022 – wissenschaftliches Programm

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O: Fachverband Oberflächenphysik

O 50: Frontiers of Electronic Structure Theory: Focus on Artificial Intelligence Applied to Real Materials 2

O 50.12: Vortrag

Mittwoch, 7. September 2022, 17:45–18:00, S054

Ab initio simulations of vibrational sum frequency generation without molecular decomposition — •Paolo Lazzaroni, Alan Lewis, and Mariana Rossi — Max Planck Institute for the Structure and Dynamics of Matter, Hamburg, Germany

Hydrogen evolution through heterogeneous catalysis is an increasingly popular solution for storage of energy generated from renewable sources, and as such is becoming a central part of green energy grids. Understanding the structure of water at solid interfaces is vital to find more efficient and cost-effective catalysts of this reaction, and sum-frequency generation spectroscopy provides a surface-specific method of investigating these structures [1]. In this work we present a new framework for ab initio calculations of the sum-frequency response which avoids the need for an arbitrary molecular decomposition of the polarizability and dipole moment. Within this approach, based on Density Functional Theory, the observables are evaluated using real space integrals directly on the whole system [2]. This allows us, for example, to unravel the effect of this decomposition on the sum-frequency response of the much-studied water/vacuum interface. This scheme also enables us, in the context of water-solid interfaces, to account explicitly for the contribution of the solid to the polarizability and dipole moment of the interface, which are commonly neglected.

[1] A. Morita, J. Hynes, J. Phys. Chem. B 106, 673 (2002)

[2] H. Shang et al, New J. Phys. 20, 073040 (2018)