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Title: A fast scheme to calculate electronic couplings between P3HT polymer units using diabatic orbitals for charge transfer dynamics simulations

We propose a fast and accurate calculation method to compute the electronic couplings between molecular units in a thiophene-ring-based polymer chain mimicking a real organic semiconducting polymer, poly(3-hexylthiophene). Through a unit block diabatization scheme, the method employed minimal number of diabatic orbitals to compute the site energies and electronic couplings, which were validated by comparing with benchmark density functional theory calculations. In addition, by using the obtained electronic couplings, a quantum dynamics simulation was carried out to propagate a hole initially localized in a thiophene-ring unit of the polymer chain. Here, this work establishes a simple, efficient, and robust means for the simulation of electron or hole transfer processes in organic semiconducting materials, an important capability for study and understanding of the class of organic optoelectronic and photovoltaic materials.
Authors:
ORCiD logo [1] ;  [1] ; ORCiD logo [2] ; ORCiD logo [3] ; ORCiD logo [3]
  1. Tennessee Technological Univ., Cookeville, TN (United States). Dept. of Chemistry
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center of Nanophase Materials Sciences & Computational Sciences and Engineering Division
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center of Nanophase Materials Sciences & Computational Sciences and Engineering Division
Publication Date:
Grant/Contract Number:
AC05-00OR22725
Type:
Accepted Manuscript
Journal Name:
Journal of Computational Chemistry
Additional Journal Information:
Journal Volume: 40; Journal Issue: 2; Journal ID: ISSN 0192-8651
Publisher:
Wiley
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; band structure; electronic structure; quantum dynamics; DFT; conducting polymers
OSTI Identifier:
1488703
Alternate Identifier(s):
OSTI ID: 1485692

Yu, Tao, Fabunmi, Florence, Huang, Jingsong, Sumpter, Bobby G., and Jakowski, Jacek. A fast scheme to calculate electronic couplings between P3HT polymer units using diabatic orbitals for charge transfer dynamics simulations. United States: N. p., Web. doi:10.1002/jcc.25749.
Yu, Tao, Fabunmi, Florence, Huang, Jingsong, Sumpter, Bobby G., & Jakowski, Jacek. A fast scheme to calculate electronic couplings between P3HT polymer units using diabatic orbitals for charge transfer dynamics simulations. United States. doi:10.1002/jcc.25749.
Yu, Tao, Fabunmi, Florence, Huang, Jingsong, Sumpter, Bobby G., and Jakowski, Jacek. 2018. "A fast scheme to calculate electronic couplings between P3HT polymer units using diabatic orbitals for charge transfer dynamics simulations". United States. doi:10.1002/jcc.25749.
@article{osti_1488703,
title = {A fast scheme to calculate electronic couplings between P3HT polymer units using diabatic orbitals for charge transfer dynamics simulations},
author = {Yu, Tao and Fabunmi, Florence and Huang, Jingsong and Sumpter, Bobby G. and Jakowski, Jacek},
abstractNote = {We propose a fast and accurate calculation method to compute the electronic couplings between molecular units in a thiophene-ring-based polymer chain mimicking a real organic semiconducting polymer, poly(3-hexylthiophene). Through a unit block diabatization scheme, the method employed minimal number of diabatic orbitals to compute the site energies and electronic couplings, which were validated by comparing with benchmark density functional theory calculations. In addition, by using the obtained electronic couplings, a quantum dynamics simulation was carried out to propagate a hole initially localized in a thiophene-ring unit of the polymer chain. Here, this work establishes a simple, efficient, and robust means for the simulation of electron or hole transfer processes in organic semiconducting materials, an important capability for study and understanding of the class of organic optoelectronic and photovoltaic materials.},
doi = {10.1002/jcc.25749},
journal = {Journal of Computational Chemistry},
number = 2,
volume = 40,
place = {United States},
year = {2018},
month = {12}
}

Works referenced in this record:

Self�Consistent Molecular Orbital Methods. XII. Further Extensions of Gaussian�Type Basis Sets for Use in Molecular Orbital Studies of Organic Molecules
journal, March 1972
  • Hehre, W. J.; Ditchfield, R.; Pople, J. A.
  • The Journal of Chemical Physics, Vol. 56, Issue 5, p. 2257-2261
  • DOI: 10.1063/1.1677527