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 50.8: Vortrag

Mittwoch, 7. September 2022, 16:45–17:00, S054

Incorporating First-Principles Electronic Friction in Instanton Rate Theory — •Yair Litman¹, Eszter S. Pos¹, Connor L. Box², Rocco Martinazzo³, Reinhard J. Maurer², and Mariana Rossi¹ — ¹MPI for the Structure and Dynamics of Matter, Hamburg, Germany. — ²Department of Chemistry, University of Warwick, Coventry, United Kingdom — ³Department of Chemistry, Università degli Studi di Milano, Milano, Italy

Reactions involving impurities in bulk metals are ubiquitous in a wide range of technological applications. The theoretical modelling of such reactions present a challenge for theory because nuclear quantum effects (NQEs) can play a prominent role and the coupling of the atomic motion with the electrons in the metal gives rise to important non-adiabatic effects (NAEs). In this work, we present a theoretical framework for the calculation of reaction rates capable of capturing both NQEs and NAEs for high-dimension realistic systems [1,2]. This is achieved by combining the ring polymer instanton (RPI) formalism with ab initio electronic friction from Ref. [3]. We derive equations that incorporate the spatial and frequency dependence of electronic friction, and name the new method RPI with explicit friction (RPI-EF). We validate RPI-EF against numerically exact results and find, quantitatively, how the friction modifies reaction rates and tunnelling pathways. Finally, we present ab initio results for H-hopping in selected bulk metals. [1] Y. Litman, E. S. Pós, C. L. Box, R. Martinazzo, R. J. Maurer, and M. Rossi, JCP 156, 194106 (2022) [2] id. JCP 156, 194107 (2022) [3] M. Head-Gordon, J. C. Tully, JCP 96, 3939 (1992).