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Non-Adiabatic Molecular Dynamics and Quantum Solvent Effects

  • Conference paper
Advanced Topics in Theoretical Chemical Physics

Part of the book series: Progress in Theoretical Chemistry and Physics ((PTCP,volume 12))

Abstract

Three novel approaches extending quantum-classical non-adiabatic (NA) molecular dynamics (MD) to include quantum effects of solvent environments are described. In a standard NA-MD the solute subsystem is treated quantum mechanically, while the larger solvent part of a system is treated classically. The three novel approaches presented here are based on the Bohmian formulation of quantum mechanics, the stochastic Schrodinger equation for the evolution of open quantum systems and the quantized Hamilton dynamics generalization of classical mechanics. The approaches extend the standard NA-MD to incorporate the following quantum effects of the solvent. 1. Branching, i.e., the ability of solvent quantum wave packets to split and follow asymptotically diverging trajectories correlated with different quantum states of the solute. 2. Decoherence, i.e., loss of quantum interference within the solute subsystem induced by the diverging solvent trajectories. 3. Zero point energy that contributes to NA coupling and must be preserved during the energy exchange between solvent and solute degrees of freedom. The Bohmian quantum-classical mechanics, stochastic mean-field and quantized mean-field approximations incorporate the quantum solvent effects into the standard quantum-classical NA-MD in a straightforward and efficient way that can be easily applied to quantum dynamics of condensed phase chemical systems.

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Authors and Affiliations

  1. Department of Chemistry, University of Washington, Seattle, WA, 98195-1700, USA

    Oleg V. Prezhdo & Craig Brooksby

Authors
  1. Oleg V. Prezhdo
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  2. Craig Brooksby
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Editor information

Editors and Affiliations

  1. Laboratoire de Chimie Physique, Université Pierre et Marie Curie, Paris, France

    Jean Maruani (Director of Research at CNRS, President of CMOA) (Director of Research at CNRS, President of CMOA)

  2. Laboratoire de Photophysique Moléculaire, Université Paris-Sud, Orsay, France

    Roland Lefebvre

  3. Department of Quantum Chemistry, University of Uppsala, Sweden

    Erkki J. Brändas

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Prezhdo, O.V., Brooksby, C. (2003). Non-Adiabatic Molecular Dynamics and Quantum Solvent Effects. In: Maruani, J., Lefebvre, R., Brändas, E.J. (eds) Advanced Topics in Theoretical Chemical Physics. Progress in Theoretical Chemistry and Physics, vol 12. Springer, Dordrecht. https://doi.org/10.1007/978-94-017-0635-3_12

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  • DOI: https://doi.org/10.1007/978-94-017-0635-3_12

  • Publisher Name: Springer, Dordrecht

  • Print ISBN: 978-90-481-6401-1

  • Online ISBN: 978-94-017-0635-3

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