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+The performance of various hybrid density functionals is assessed for 105 singlet and 105 corresponding triplet vertical excitation energies from the QUEST database. The overall lowest mean absolute error is obtained with the local hybrid (LH) functional LH12ct-SsirPW92 with individual errors of 0.11 eV (0.11 eV) for singlet (triplet) n → π* excitations and 0.29 eV (0.17 eV) for π → π* excitations. This is slightly better than with the overall best performing global hybrid M06-2X [n → π*: 0.13 eV (0.17 eV), π → π*: 0.30 eV (0.20 eV)], while most other global and range-separated hybrids and some LHs suffer from the “triplet problem” of time-dependent density functional theory. This is exemplified by correlating the errors for singlet and triplet excitations on a state-by-state basis. The excellent performance of LHs based on a common local mixing function, i.e., an LMF constructed from the spin-summed rather than the spin-resolved semilocal quantities, is systematically investigated by the introduction of a spin-channel interpolation scheme that allows us to continuously modulate the fraction of opposite-spin terms used in the LMF. The correlation of triplet and singlet errors is systematically improved for the n → π* excitations when larger fractions of the opposite-spin-channel are used in the LMF, whereas this effect is limited for the π → π* excitations. This strongly supports a previously made hypothesis that attributes the excellent performance of LHs based on a common LMF to cross-spin-channel nondynamical correlation terms.
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