  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
H$_2$ and H$_2^+$, 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 H$_2$ and H$_2^{+}$, ZRPS yields a remarkable and
consistent improvement over other density functionals across various chemical
environments from weak to strong correlation.

Materials Science;Chemical Physics