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Performance and Self-Consistency of the Generalized Dielectric Dependent Hybrid Functional

Journal Article · · Journal of Chemical Theory and Computation
 [1];  [2];  [2];  [2]
  1. Univ. of Chicago, Chicago, IL (United States)
  2. Univ. of Chicago, Chicago, IL (United States); Argonne National Lab. (ANL), Lemont, IL (United States)
+ Show Author Affiliations
Here, we analyze the performance of the recently proposed screened exchange constant functional (SX) on the GW100 test set, and we discuss results obtained at different levels of self-consistency. The SX functional is a generalization of dielectric dependent hybrid functionals to finite systems; it is nonempirical and depends on the average screening of the exchange interaction. We compare results for ionization potentials obtained with SX to those of CCSD(T) calculations and experiments, and we find excellent agreement, on par with recent state of the art methods based on many body perturbation theory. Applying SX perturbatively to correct PBE eigenvalues yields improved results in most cases, except for ionic molecules, for which wave function self-consistency is instead crucial. Calculations where wave functions and the screened exchange constant (αSX) are determined self-consistently, and those where αSX is fixed to the value determined within PBE, yield results of comparable accuracy. Perturbative G0W0 corrections of eigenvalues obtained with self-consistent αSX are small on average, for all molecules in the GW100 test set.
Research Organization:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1389645
Journal Information:
Journal of Chemical Theory and Computation, Journal Name: Journal of Chemical Theory and Computation Journal Issue: 7 Vol. 13; ISSN 1549-9618
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

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Cited By (7)

Quantum Embedding Theory for Strongly-correlated States in Materials text January 2021
Dielectric Screening Meets Optimally Tuned Density Functionals journal April 2018
Screened hybrid meta-GGA exchange–correlation functionals for extended systems journal January 2019
Combining Landau–Zener theory and kinetic Monte Carlo sampling for small polaron mobility of doped BiVO 4 from first-principles journal January 2018
Efficient lattice constants and energy bandgaps for condensed systems from a meta-GGA level screened range-separated hybrid functional journal September 2018
Dielectric-dependent hybrid functionals for heterogeneous materials journal July 2019
Dielectric dependent hybrid functionals for heterogeneous materials text January 2019

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