Generalized Optimized Effective Potential for Orbital Functionals and SelfConsistent Calculation of Random Phase Approximations
Abstract
A new selfconsistent procedure for calculating the total energy with an orbitaldependent density functional approximation (DFA), the generalized optimized effective potential (GOEP), is developed in the present work. The GOEP is a nonlocal Hermitian potential that delivers the sets of occupied and virtual orbitals and minimizes the total energy. The GOEP optimization leads to the same minimum as does the orbital optimization. The GOEP method is promising as an effective optimization approach for orbitaldependent functionals, as demonstrated for the selfconsistent calculations of the random phase approximation (RPA) to the correlation functionals in the particle–hole (ph) and particle–particle (pp) channels. The results show that the accuracy in describing the weakly interacting van der Waals systems is significantly improved in the selfconsistent calculations. In particular, the important single excitations contribution in nonselfconsistent RPA calculations can be captured selfconsistently through the GOEP optimization, leading to orbital renormalization, without using the single excitations in the energy functional.
 Authors:

 Duke Univ., Durham, NC (United States). Dept. of Chemistry
 Publication Date:
 Research Org.:
 Energy Frontier Research Centers (EFRC) (United States). Center for the Computational Design of Functional Layered Materials (CCDM)
 Sponsoring Org.:
 USDOE Office of Science (SC), Basic Energy Sciences (BES)
 OSTI Identifier:
 1469927
 Grant/Contract Number:
 SC0012575
 Resource Type:
 Accepted Manuscript
 Journal Name:
 Journal of Physical Chemistry Letters
 Additional Journal Information:
 Journal Volume: 8; Journal Issue: 19; Related Information: CCDM partners with Temple University (lead); Brookhaven National Laboratory; Drexel University; Duke University; North Carolina State University; Northeastern University; Princeton University; Rice University; University of Pennsylvania; Journal ID: ISSN 19487185
 Publisher:
 American Chemical Society
 Country of Publication:
 United States
 Language:
 English
 Subject:
 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; catalysis (heterogeneous); solar (photovoltaic); energy storage (including batteries and capacitors); hydrogen and fuel cells; defects; mechanical behavior; materials and chemistry by design; synthesis (novel materials)
Citation Formats
Jin, Ye, Zhang, Du, Chen, Zehua, Su, Neil Qiang, and Yang, Weitao. Generalized Optimized Effective Potential for Orbital Functionals and SelfConsistent Calculation of Random Phase Approximations. United States: N. p., 2017.
Web. https://doi.org/10.1021/acs.jpclett.7b02165.
Jin, Ye, Zhang, Du, Chen, Zehua, Su, Neil Qiang, & Yang, Weitao. Generalized Optimized Effective Potential for Orbital Functionals and SelfConsistent Calculation of Random Phase Approximations. United States. https://doi.org/10.1021/acs.jpclett.7b02165
Jin, Ye, Zhang, Du, Chen, Zehua, Su, Neil Qiang, and Yang, Weitao. Tue .
"Generalized Optimized Effective Potential for Orbital Functionals and SelfConsistent Calculation of Random Phase Approximations". United States. https://doi.org/10.1021/acs.jpclett.7b02165. https://www.osti.gov/servlets/purl/1469927.
@article{osti_1469927,
title = {Generalized Optimized Effective Potential for Orbital Functionals and SelfConsistent Calculation of Random Phase Approximations},
author = {Jin, Ye and Zhang, Du and Chen, Zehua and Su, Neil Qiang and Yang, Weitao},
abstractNote = {A new selfconsistent procedure for calculating the total energy with an orbitaldependent density functional approximation (DFA), the generalized optimized effective potential (GOEP), is developed in the present work. The GOEP is a nonlocal Hermitian potential that delivers the sets of occupied and virtual orbitals and minimizes the total energy. The GOEP optimization leads to the same minimum as does the orbital optimization. The GOEP method is promising as an effective optimization approach for orbitaldependent functionals, as demonstrated for the selfconsistent calculations of the random phase approximation (RPA) to the correlation functionals in the particle–hole (ph) and particle–particle (pp) channels. The results show that the accuracy in describing the weakly interacting van der Waals systems is significantly improved in the selfconsistent calculations. In particular, the important single excitations contribution in nonselfconsistent RPA calculations can be captured selfconsistently through the GOEP optimization, leading to orbital renormalization, without using the single excitations in the energy functional.},
doi = {10.1021/acs.jpclett.7b02165},
journal = {Journal of Physical Chemistry Letters},
number = 19,
volume = 8,
place = {United States},
year = {2017},
month = {9}
}
Web of Science
Works referencing / citing this record:
Variational generalized KohnSham approach combining the randomphaseapproximation and Green'sfunction methods
journal, January 2019
 Voora, Vamsee K.; Balasubramani, Sree Ganesh; Furche, Filipp
 Physical Review A, Vol. 99, Issue 1