Accurate double excitations from ensemble density functional calculations
Francisca Sagredo, Kieron Burke
The recent use of a new ensemble in density functional theory (DFT) to produce direct corrections to the Kohn-Sham transitions yields the elusive double excitations that are missed by time-dependent DFT (TDDFT) with the standard adiabatic approximation. But accuracies are lower than for single excitations, and formal arguments about TDDFT suggest that a correction kernel is needed. In principle, ensemble DFT with direct corrections at the exchange level must yield accurate doubles in the weakly correlated limit. We illustrate with exact calculations and analytic results on the Hubbard dimer. We also explain the error in formal arguments in TDDFT.
arXiv:1806.03392•The Journal of Chemical Physics•Oct 2, 2018•46 citations