Article (Scientific journals)
Beyond the random-phase approximation for the electron correlation energy: The importance of single excitations
Ren, X.; Tkatchenko, Alexandre; Rinke, P. et al.
2011In Physical Review Letters, 106 (15)
Peer reviewed
 

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Keywords :
Correlation energy; Electron correlation energy; Exact exchange; Exchange-correlation functionals; Exchange-correlations; Hartree-fock; Intermolecular interactions; Kohn-Sham orbitals; Noncovalent; Orbitals; Random phase approximations; Random-phase approximation; Single excitation; Total energy; Density functional theory; Electron correlations; Electron density measurement; Standards; Correlation methods
Abstract :
[en] The random-phase approximation (RPA) for the electron correlation energy, combined with the exact-exchange (EX) energy, represents the state-of-the-art exchange-correlation functional within density-functional theory. However, the standard RPA practice-evaluating both the EX and the RPA correlation energies using Kohn-Sham (KS) orbitals from local or semilocal exchange-correlation functionals-leads to a systematic underbinding of molecules and solids. Here we demonstrate that this behavior can be corrected by adding a "single excitation" contribution, so far not included in the standard RPA scheme. A similar improvement can also be achieved by replacing the non-self-consistent EX total energy by the corresponding self-consistent Hartree-Fock total energy, while retaining the RPA correlation energy evaluated using KS orbitals. Both schemes achieve chemical accuracy for a standard benchmark set of noncovalent intermolecular interactions. © 2011 American Physical Society.
Disciplines :
Physics
Identifiers :
eid=2-s2.0-79960624488
Author, co-author :
Ren, X.;  Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195, Berlin, Germany
Tkatchenko, Alexandre ;  Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195, Berlin, Germany
Rinke, P.;  Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195, Berlin, Germany
Scheffler, M.;  Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195, Berlin, Germany
External co-authors :
yes
Title :
Beyond the random-phase approximation for the electron correlation energy: The importance of single excitations
Publication date :
2011
Journal title :
Physical Review Letters
ISSN :
0031-9007
Volume :
106
Issue :
15
Peer reviewed :
Peer reviewed
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