skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

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:
; ;  [1]
  1. Department of Chemistry, University of Rochester, Rochester, New York 14627 (United States)
Publication Date:
OSTI Identifier:
22251516
Resource Type:
Journal Article
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 139; Journal Issue: 17; Other Information: (c) 2013 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0021-9606
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

Citation Formats

Wang, Linjun, Chen, Liping, Prezhdo, Oleg V., E-mail: linjun.wang@rochester.edu, E-mail: oleg.prezhdo@rochester.edu, Akimov, Alexey V., and Chemistry Department, Brookhaven National Laboratory, Upton, New York 11973-5000. Quantized Hamiltonian dynamics captures the low-temperature regime of charge transport in molecular crystals. United States: N. p., 2013. Web. doi:10.1063/1.4828863.
Wang, Linjun, Chen, Liping, Prezhdo, Oleg V., E-mail: linjun.wang@rochester.edu, E-mail: oleg.prezhdo@rochester.edu, Akimov, Alexey V., & Chemistry Department, Brookhaven National Laboratory, Upton, New York 11973-5000. Quantized Hamiltonian dynamics captures the low-temperature regime of charge transport in molecular crystals. United States. https://doi.org/10.1063/1.4828863
Wang, Linjun, Chen, Liping, Prezhdo, Oleg V., E-mail: linjun.wang@rochester.edu, E-mail: oleg.prezhdo@rochester.edu, Akimov, Alexey V., and Chemistry Department, Brookhaven National Laboratory, Upton, New York 11973-5000. 2013. "Quantized Hamiltonian dynamics captures the low-temperature regime of charge transport in molecular crystals". United States. https://doi.org/10.1063/1.4828863.
@article{osti_22251516,
title = {Quantized Hamiltonian dynamics captures the low-temperature regime of charge transport in molecular crystals},
author = {Wang, Linjun and Chen, Liping and Prezhdo, Oleg V., E-mail: linjun.wang@rochester.edu, E-mail: oleg.prezhdo@rochester.edu and Akimov, Alexey V. and Chemistry Department, Brookhaven National Laboratory, Upton, New York 11973-5000},
abstractNote = {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.},
doi = {10.1063/1.4828863},
url = {https://www.osti.gov/biblio/22251516}, journal = {Journal of Chemical Physics},
issn = {0021-9606},
number = 17,
volume = 139,
place = {United States},
year = {Thu Nov 07 00:00:00 EST 2013},
month = {Thu Nov 07 00:00:00 EST 2013}
}