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

Journal Article · · Physical Review. X
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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.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE National Nuclear Security Administration (NNSA)
Grant/Contract Number:
AC02-06CH11357; AC02-05CH11231; AC52-06NA25396
OSTI ID:
1328479
Alternate ID(s):
OSTI ID: 1335882
Journal Information:
Physical Review. X, Journal Name: Physical Review. X Vol. 6 Journal Issue: 4; ISSN 2160-3308
Publisher:
American Physical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 60 works
Citation information provided by
Web of Science

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