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Title: Mixed quantum-classical simulations of charge transport in organic materials: Numerical benchmark of the Su-Schrieffer-Heeger model

Abstract

The electron-phonon coupling is critical in determining the intrinsic charge carrier and exciton transport properties in organic materials. In this study, we consider a Su-Schrieffer-Heeger (SSH) model for molecular crystals, and perform numerical benchmark studies for different strategies of simulating the mixed quantum-classical dynamics. These methods, which differ in the selection of initial conditions and the representation used to solve the time evolution of the quantum carriers, are shown to yield similar equilibrium diffusion properties. A hybrid approach combining molecular dynamics simulations of nuclear motion and quantum-chemical calculations of the electronic Hamiltonian at each geometric configuration appears as an attractive strategy to model charge dynamics in large size systems ''on the fly,'' yet it relies on the assumption that the quantum carriers do not impact the nuclear dynamics. We find that such an approximation systematically results in overestimated charge-carrier mobilities, with the associated error being negligible when the room-temperature mobility exceeds {approx}4.8 cm{sup 2}/Vs ({approx}0.14 cm{sup 2}/Vs) in one-dimensional (two-dimensional) crystals.

Authors:
;  [1]; ;  [2]
  1. Laboratory for Chemistry of Novel Materials, University of Mons, Place du Parc 20, B-7000 Mons (Belgium)
  2. State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences, Zhongguancun, 100190 Beijing (China)
Publication Date:
OSTI Identifier:
21560310
Resource Type:
Journal Article
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 134; Journal Issue: 24; Other Information: DOI: 10.1063/1.3604561; (c) 2011 American Institute of Physics; Journal ID: ISSN 0021-9606
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; APPROXIMATIONS; BENCHMARKS; CARRIER MOBILITY; CHARGE CARRIERS; CHARGE EXCHANGE; CHARGE TRANSPORT; DIFFUSION; ELECTRON-PHONON COUPLING; EQUILIBRIUM; ERRORS; EXCITONS; HAMILTONIANS; MOLECULAR CRYSTALS; MOLECULAR DYNAMICS METHOD; ONE-DIMENSIONAL CALCULATIONS; ORGANIC COMPOUNDS; ORGANIC MATTER; SIMULATION; CALCULATION METHODS; COUPLING; CRYSTALS; MATHEMATICAL OPERATORS; MATTER; MOBILITY; QUANTUM OPERATORS; QUASI PARTICLES

Citation Formats

Linjun, Wang, Beljonne, David, Liping, Chen, and Qiang, Shi. Mixed quantum-classical simulations of charge transport in organic materials: Numerical benchmark of the Su-Schrieffer-Heeger model. United States: N. p., 2011. Web. doi:10.1063/1.3604561.
Linjun, Wang, Beljonne, David, Liping, Chen, & Qiang, Shi. Mixed quantum-classical simulations of charge transport in organic materials: Numerical benchmark of the Su-Schrieffer-Heeger model. United States. https://doi.org/10.1063/1.3604561
Linjun, Wang, Beljonne, David, Liping, Chen, and Qiang, Shi. 2011. "Mixed quantum-classical simulations of charge transport in organic materials: Numerical benchmark of the Su-Schrieffer-Heeger model". United States. https://doi.org/10.1063/1.3604561.
@article{osti_21560310,
title = {Mixed quantum-classical simulations of charge transport in organic materials: Numerical benchmark of the Su-Schrieffer-Heeger model},
author = {Linjun, Wang and Beljonne, David and Liping, Chen and Qiang, Shi},
abstractNote = {The electron-phonon coupling is critical in determining the intrinsic charge carrier and exciton transport properties in organic materials. In this study, we consider a Su-Schrieffer-Heeger (SSH) model for molecular crystals, and perform numerical benchmark studies for different strategies of simulating the mixed quantum-classical dynamics. These methods, which differ in the selection of initial conditions and the representation used to solve the time evolution of the quantum carriers, are shown to yield similar equilibrium diffusion properties. A hybrid approach combining molecular dynamics simulations of nuclear motion and quantum-chemical calculations of the electronic Hamiltonian at each geometric configuration appears as an attractive strategy to model charge dynamics in large size systems ''on the fly,'' yet it relies on the assumption that the quantum carriers do not impact the nuclear dynamics. We find that such an approximation systematically results in overestimated charge-carrier mobilities, with the associated error being negligible when the room-temperature mobility exceeds {approx}4.8 cm{sup 2}/Vs ({approx}0.14 cm{sup 2}/Vs) in one-dimensional (two-dimensional) crystals.},
doi = {10.1063/1.3604561},
url = {https://www.osti.gov/biblio/21560310}, journal = {Journal of Chemical Physics},
issn = {0021-9606},
number = 24,
volume = 134,
place = {United States},
year = {2011},
month = {6}
}