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Nuclear quantum effects in electronic (non)adiabatic dynamics

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Abstract

Trajectory-based approaches to excited-state, nonadiabatic dynamics are promising simulation techniques to describe the response of complex molecular systems upon photo-excitation. They provide an approximate description of the coupled quantum dynamics of electrons and nuclei trying to access systems of growing complexity. The central question in the design of those approximations is a proper accounting of the coupling electron-nuclei and of the quantum features of the problem. In this paper, we approach the problem in the framework of the exact factorization of the electron-nuclear wavefunction, re-deriving and improving the coupled-trajectory mixed quantum-classical (CT-MQC) algorithm recently developed to solve the exact-factorization equations. In particular, a procedure to include quantum nuclear effects in CT-MQC is derived, and tested on a model system in different regimes.

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Authors and Affiliations

  1. Laboratoire de Chimie Physique, UMR 8000 CNRS/University Paris-Sud, 91405, Orsay, France

    Federica Agostini

  2. IBM Research GmbH, Zürich Research Laboratory, 8803, Rüschlikon, Switzerland

    Ivano Tavernelli

  3. Institute for Applied Computing “Mauro Picone” (IAC), CNR, Via dei Taurini 19, 00185, Roma, Italy

    Giovanni Ciccotti

  4. School of Physics, University College of Dublin UCD – Belfield, Dublin 4, Ireland

    Giovanni Ciccotti

  5. Università di Roma La Sapienza, P.le A. Moro 5, 00185, Roma, Italy

    Giovanni Ciccotti

Authors
  1. Federica Agostini
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  2. Ivano Tavernelli
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  3. Giovanni Ciccotti
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Correspondence to Federica Agostini.

Additional information

Contribution to the Topical Issue “Special issue in honor of Hardy Gross”, edited by C.A. Ullrich, F.M.S. Nogueira, A. Rubio, and M.A.L. Marques.

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Agostini, F., Tavernelli, I. & Ciccotti, G. Nuclear quantum effects in electronic (non)adiabatic dynamics. Eur. Phys. J. B 91, 139 (2018). https://doi.org/10.1140/epjb/e2018-90144-3

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  • DOI: https://doi.org/10.1140/epjb/e2018-90144-3

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