title: Quantized Hamiltonian dynamics captures the low-temperature regime of charge transport in molecular crystals.
abstract: 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.affiliation: Department of Chemistry, University of Rochester, Rochester, New York 14627, USA.
authors.forename: Linjun
authors.initials: L
authors.lastname: Wang
authors.forename: Alexey V
authors.initials: AV
authors.lastname: Akimov
authors.forename: Liping
authors.initials: L
authors.lastname: Chen
authors.forename: Oleg V
authors.initials: OV
authors.lastname: Prezhdo