Singles correlation energy contributions in solids

0446834 - ÚFCH JH 2016 RIV US eng J - Článek v odborném periodiku
Klimeš, Jiří - Kaltak, M. - Maggio, E. - Kresse, G.
Singles correlation energy contributions in solids.
Journal of Chemical Physics. Roč. 143, č. 10 (2015), s. 102816. ISSN 0021-9606. E-ISSN 1089-7690
Grant ostatní: GA MŠk(CZ) LM2010005
Institucionální podpora: RVO:61388955
Klíčová slova: Density functional theory * Green's function methods * Lattice constants
Kód oboru RIV: CF - Fyzikální chemie a teoretická chemie
Impakt faktor: 2.894, rok: 2015

The random phase approximation to the correlation energy often yields highly accurate results for condensed matter systems. However, ways how to improve its accuracy are being sought and here we explore the relevance of singles contributions for prototypical solid state systems. We set out with a derivation of the random phase approximation using the adiabatic connection and fluctuation dissipation theorem, but contrary to the most commonly used derivation, the density is allowed to vary along the coupling constant integral. This yields results closely paralleling standard perturbation theory. We re-derive the standard singles of Görling-Levy perturbation theory [A. Görling and M. Levy, Phys. Rev. A 50, 196 (1994)], highlight the analogy of our expression to the renormalized singles introduced by Ren and coworkers [Phys. Rev. Lett. 106, 153003 (2011)], and introduce a new approximation for the singles using the density matrix in the random phase approximation. We discuss the physical relevance and importance of singles alongside illustrative examples of simple weakly bonded systems, including rare gas solids (Ne, Ar, Xe), ice, adsorption of water on NaCl, and solid benzene. The effect of singles on covalently and metallically bonded systems is also discussed.
Trvalý link: http://hdl.handle.net/11104/0248798