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Title: Quantized Hamiltonian dynamics captures the low-temperature regime of charge transport in molecular crystals

The quantized Hamiltonian dynamics (QHD) theory provides a hierarchy of approximations to quantum dynamics in the Heisenberg representation. We apply the first-order QHD to study charge transport in molecular crystals and find that the obtained equations of motion coincide with the Ehrenfest theory, which is the most widely used mixed quantum-classical approach. Quantum initial conditions required for the QHD variables make the dynamics surpass Ehrenfest. Most importantly, the first-order QHD already captures the low-temperature regime of charge transport, as observed experimentally. We expect that simple extensions to higher-order QHDs can efficiently represent other quantum effects, such as phonon zero-point energy and loss of coherence in the electronic subsystem caused by phonons.
Authors:
; ;  [1] ;  [1] ;  [2]
  1. Department of Chemistry, University of Rochester, Rochester, New York 14627 (United States)
  2. (United States)
Publication Date:
OSTI Identifier:
22251516
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 139; Journal Issue: 17; Other Information: (c) 2013 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
73 NUCLEAR PHYSICS AND RADIATION PHYSICS; 74 ATOMIC AND MOLECULAR PHYSICS; APPROXIMATIONS; CAPTURE; CHARGE TRANSPORT; EQUATIONS OF MOTION; HAMILTONIANS; HEISENBERG PICTURE; MOLECULAR CRYSTALS; PHONONS