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Title: Generalization of Dielectric-Dependent Hybrid Functionals to Finite Systems

Abstract

The accurate prediction of electronic and optical properties of molecules and solids is a persistent challenge for methods based on density functional theory. We propose a generalization of dielectric-dependent hybrid functionals to finite systems where the definition of the mixing fraction of exact and semilocal exchange is physically motivated, nonempirical, and system dependent. The proposed functional yields ionization potentials, and fundamental and optical gaps of many, diverse molecular systems in excellent agreement with experiments, including organic and inorganic molecules and semiconducting nanocrystals. As a result, we further demonstrate that this hybrid functional gives the correct alignment between energy levels of the exemplary TTF-TCNQ donor-acceptor system.

Authors:
; ; ;
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1328479
Alternate Identifier(s):
OSTI ID: 1335882
Grant/Contract Number:  
AC02-06CH11357; AC02-05CH11231; AC52-06NA25396
Resource Type:
Published Article
Journal Name:
Physical Review. X
Additional Journal Information:
Journal Name: Physical Review. X Journal Volume: 6 Journal Issue: 4; Journal ID: ISSN 2160-3308
Publisher:
American Physical Society
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS

Citation Formats

Brawand, Nicholas P., Vörös, Márton, Govoni, Marco, and Galli, Giulia. Generalization of Dielectric-Dependent Hybrid Functionals to Finite Systems. United States: N. p., 2016. Web. doi:10.1103/PhysRevX.6.041002.
Brawand, Nicholas P., Vörös, Márton, Govoni, Marco, & Galli, Giulia. Generalization of Dielectric-Dependent Hybrid Functionals to Finite Systems. United States. doi:10.1103/PhysRevX.6.041002.
Brawand, Nicholas P., Vörös, Márton, Govoni, Marco, and Galli, Giulia. Tue . "Generalization of Dielectric-Dependent Hybrid Functionals to Finite Systems". United States. doi:10.1103/PhysRevX.6.041002.
@article{osti_1328479,
title = {Generalization of Dielectric-Dependent Hybrid Functionals to Finite Systems},
author = {Brawand, Nicholas P. and Vörös, Márton and Govoni, Marco and Galli, Giulia},
abstractNote = {The accurate prediction of electronic and optical properties of molecules and solids is a persistent challenge for methods based on density functional theory. We propose a generalization of dielectric-dependent hybrid functionals to finite systems where the definition of the mixing fraction of exact and semilocal exchange is physically motivated, nonempirical, and system dependent. The proposed functional yields ionization potentials, and fundamental and optical gaps of many, diverse molecular systems in excellent agreement with experiments, including organic and inorganic molecules and semiconducting nanocrystals. As a result, we further demonstrate that this hybrid functional gives the correct alignment between energy levels of the exemplary TTF-TCNQ donor-acceptor system.},
doi = {10.1103/PhysRevX.6.041002},
journal = {Physical Review. X},
number = 4,
volume = 6,
place = {United States},
year = {2016},
month = {10}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1103/PhysRevX.6.041002

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Cited by: 8 works
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    Works referencing / citing this record:

    Dielectric-dependent hybrid functionals for heterogeneous materials
    journal, July 2019