Coupled-Trajectory Quantum-Classical Approach to Electronic Decoherence in Nonadiabatic Processes

Seung Kyu Min, Federica Agostini, and E. K. U. Gross
Phys. Rev. Lett. 115, 073001 – Published 10 August 2015
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Abstract

We present a novel quantum-classical approach to nonadiabatic dynamics, deduced from the coupled electronic and nuclear equations in the framework of the exact factorization of the electron-nuclear wave function. The method is based on the quasiclassical interpretation of the nuclear wave function, whose phase is related to the classical momentum and whose density is represented in terms of classical trajectories. In this approximation, electronic decoherence is naturally induced as an effect of the coupling to the nuclei and correctly reproduces the expected quantum behavior. Moreover, the splitting of the nuclear wave packet is captured as a consequence of the correct approximation of the time-dependent potential of the theory. This new approach offers a clear improvement over Ehrenfest-like dynamics. The theoretical derivation presented in this Letter is supported by numerical results that are compared to quantum mechanical calculations.

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  • Received 1 April 2015

DOI:https://doi.org/10.1103/PhysRevLett.115.073001

© 2015 American Physical Society

Authors & Affiliations

Seung Kyu Min1,2, Federica Agostini1, and E. K. U. Gross1

  • 1Max-Planck Institut für Mikrostrukturphysik, Weinberg 2, D-06120 Halle, Germany
  • 2Department of Chemistry, School of Natural Science, Ulsan National Institute of Science and Technology (UNIST), Ulsan 689-798, Korea

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Issue

Vol. 115, Iss. 7 — 14 August 2015

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