Article (Scientific journals)
Quantitative Prediction of Optical Absorption in Molecular Solids from an Optimally Tuned Screened Range-Separated Hybrid Functional
Manna, Arun; Refaely-Abramson, Sivan; Reilly, Anthony et al.
2018In Journal of Chemical Theory and Computation, 14, p. 11
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Abstract :
[en] We show that fundamental gaps and optical spectra of molecular solids can be predicted quantitatively and nonempirically within the framework of time-dependent density functional theory (TDDFT) using the recently developed optimally tuned screened range-separated hybrid (OT-SRSH) functional approach. In this scheme, the electronic structure of the gas-phase molecule is determined by optimal tuning of the range-separation parameter in a range-separated hybrid functional. Screening and polarization in the solid state are taken into account by adding long-range dielectric screening to the functional form, with the modified functional used to perform self-consistent periodic boundary calculations for the crystalline solid. We provide a comprehensive benchmark for the accuracy of our approach by considering the X23 set of molecular solids and comparing results obtained from TDDFT with those obtained from many-body perturbation theory in the GW-BSE approximation. We additionally compare results obtained from dielectric screening computed within the random-phase approximation to those obtained from the computationally more efficient many-body dispersion approach and find that this influences the fundamental gap but has little effect on the optical spectra. Our approach is therefore robust and can be used for studies of molecular solids that are typically beyond the reach of computationally more intensive methods.
Disciplines :
Physics
Author, co-author :
Manna, Arun
Refaely-Abramson, Sivan
Reilly, Anthony
Tkatchenko, Alexandre ;  University of Luxembourg > Faculty of Science, Technology and Communication (FSTC) > Physics and Materials Science Research Unit
Neaton, Jeffrey
Kronik, Leeor
External co-authors :
yes
Language :
English
Title :
Quantitative Prediction of Optical Absorption in Molecular Solids from an Optimally Tuned Screened Range-Separated Hybrid Functional
Publication date :
04 May 2018
Journal title :
Journal of Chemical Theory and Computation
ISSN :
1549-9618
eISSN :
1549-9626
Publisher :
American Chemical Society, United States - District of Columbia
Volume :
14
Pages :
11
Peer reviewed :
Peer Reviewed verified by ORBi
Focus Area :
Physics and Materials Science
Available on ORBilu :
since 01 January 2019

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