Density-functional theory for ensembles of fractionally occupied states. I. Basic formalism

Abstract
A density-functional theory for ensembles of unequally weighted states is formulated on the basis of the generalized Rayleigh-Ritz principle of the preceding paper. From this formalism, two alternative approaches to the computation of excitation energies are derived, one equivalent to the equiensemble method proposed by Theophilou [J. Phys. C 12, 5419 (1979)], the other grounded on an expression relating the excitation energies to the Kohn-Sham single-particle eigenvalues.