Abstrakti
We present a new paradigm for the design of exchange-correlation functionals in density-functional theory. Electron pairs are correlated explicitly by means of the recently developed second order Bethe-Goldstone equation (BGE2) approach. Here we propose a screened BGE2 (sBGE2) variant that efficiently regulates the coupling of a given electron pair. sBGE2 correctly dissociates H2 and H2+, a problem that has been regarded as a great challenge in density-functional theory for a long time. The sBGE2 functional is then taken as a building block for an orbital-dependent functional, termed ZRPS, which is a natural extension of the PBE0 hybrid functional. While worsening the good performance of sBGE2 in H2 and H2+, ZRPS yields a remarkable and consistent improvement over other density functionals across various chemical environments from weak to strong correlation.
Alkuperäiskieli | Englanti |
---|---|
Artikkeli | 133002 |
Sivut | 1-5 |
Julkaisu | Physical Review Letters |
Vuosikerta | 117 |
Numero | 13 |
DOI - pysyväislinkit | |
Tila | Julkaistu - 21 syysk. 2016 |
OKM-julkaisutyyppi | A1 Julkaistu artikkeli, soviteltu |