Quantum corrected Langevin dynamics for adsorbates on metal surfaces interacting with hot electrons

The Journal of Chemical Physics
Thomas Olsen, Jakob Schiotz

Abstract

We investigate the importance of including quantized initial conditions in Langevin dynamics for adsorbates interacting with a thermal reservoir of electrons. For quadratic potentials the time evolution is exactly described by a classical Langevin equation and it is shown how to rigorously obtain quantum mechanical probabilities from the classical phase space distributions resulting from the dynamics. At short time scales, classical and quasiclassical initial conditions lead to wrong results and only correctly quantized initial conditions give a close agreement with an inherently quantum mechanical master equation approach. With CO on Cu(100) as an example, we demonstrate the effect for a system with ab initio frictional tensor and potential energy surfaces and show that quantizing the initial conditions can have a large impact on both the desorption probability and the distribution of molecular vibrational states.

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Apr 7, 2010·Physical Review Letters·Thomas Olsen, Jakob Schiøtz

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Citations

Oct 15, 2010·The Journal of Chemical Physics·Thomas Olsen, Jakob Schiøtz
Nov 12, 2016·Physical Review Letters·Ken-Ichi InoueTomokazu Yasuike

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