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Title: Charge transport in nanostructured materials: Implementation and verification of constrained density functional theory

Abstract

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:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2];  [3]
  1. Univ. of Chicago, Chicago, IL (United States)
  2. Argonne National Lab. (ANL), Lemont, IL (United States)
  3. Univ. of Chicago, Chicago, IL (United States); Argonne National Lab. (ANL), Lemont, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1371760
Grant/Contract Number:
AC02-06CH11357
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Chemical Theory and Computation
Additional Journal Information:
Journal Volume: 13; Journal Issue: 6; Journal ID: ISSN 1549-9618
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

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., 2017. 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. Thu . "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 = {Thu Apr 20 00:00:00 EDT 2017},
month = {Thu Apr 20 00:00:00 EDT 2017}
}

Journal Article:
Free Publicly Available Full Text
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Cited by: 1work
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