Charge transport in nanostructured materials: Implementation and verification of constrained density functional theory
The in silico design of novel complex materials for energy conversion requires accurate, ab initio simulation of charge transport. In this work, we present an implementation of constrained density functional theory (CDFT) for the calculation of parameters for charge transport in the hopping regime. We verify our implementation against literature results for molecular systems, and we discuss the dependence of results on numerical parameters and the choice of localization potentials. In addition, we compare CDFT results with those of other commonly used methods for simulating charge transport between nanoscale building blocks. As a result, we show that some of these methods give unphysical results for thermally disordered configurations, while CDFT proves to be a viable and robust approach.
 Authors:

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;
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;
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 Univ. of Chicago, Chicago, IL (United States)
 Argonne National Lab. (ANL), Lemont, IL (United States)
 Univ. of Chicago, Chicago, IL (United States); Argonne National Lab. (ANL), Lemont, IL (United States)
 Publication Date:
 Grant/Contract Number:
 AC0206CH11357
 Type:
 Accepted Manuscript
 Journal Name:
 Journal of Chemical Theory and Computation
 Additional Journal Information:
 Journal Volume: 13; Journal Issue: 6; Journal ID: ISSN 15499618
 Publisher:
 American Chemical Society
 Research Org:
 Argonne National Lab. (ANL), Argonne, IL (United States)
 Sponsoring Org:
 USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC22)
 Country of Publication:
 United States
 Language:
 English
 Subject:
 36 MATERIALS SCIENCE
 OSTI Identifier:
 1371760
Goldey, Matthew B., Brawand, Nicholas P., Voros, Marton, and Galli, Giulia. Charge transport in nanostructured materials: Implementation and verification of constrained density functional theory. United States: N. p.,
Web. doi:10.1021/acs.jctc.7b00088.
Goldey, Matthew B., Brawand, Nicholas P., Voros, Marton, & Galli, Giulia. Charge transport in nanostructured materials: Implementation and verification of constrained density functional theory. United States. doi:10.1021/acs.jctc.7b00088.
Goldey, Matthew B., Brawand, Nicholas P., Voros, Marton, and Galli, Giulia. 2017.
"Charge transport in nanostructured materials: Implementation and verification of constrained density functional theory". United States.
doi:10.1021/acs.jctc.7b00088. https://www.osti.gov/servlets/purl/1371760.
@article{osti_1371760,
title = {Charge transport in nanostructured materials: Implementation and verification of constrained density functional theory},
author = {Goldey, Matthew B. and Brawand, Nicholas P. and Voros, Marton and Galli, Giulia},
abstractNote = {The in silico design of novel complex materials for energy conversion requires accurate, ab initio simulation of charge transport. In this work, we present an implementation of constrained density functional theory (CDFT) for the calculation of parameters for charge transport in the hopping regime. We verify our implementation against literature results for molecular systems, and we discuss the dependence of results on numerical parameters and the choice of localization potentials. In addition, we compare CDFT results with those of other commonly used methods for simulating charge transport between nanoscale building blocks. As a result, we show that some of these methods give unphysical results for thermally disordered configurations, while CDFT proves to be a viable and robust approach.},
doi = {10.1021/acs.jctc.7b00088},
journal = {Journal of Chemical Theory and Computation},
number = 6,
volume = 13,
place = {United States},
year = {2017},
month = {4}
}