Density Functional Theory: Excited States and Spin Annihilation

Cramer, C. J.; Dulles, F. J.; Giesen, D. J.; Almlöf, J.
Chem. Phys. Lett. 1995, 245, 165.

A spin-annihilation technique for a single determinant formed from Kohn-Sham orbitals is described for the calculation of excited state singlet energies. This procedure accurately calculates the 1¹Bu <-- 1¹Ag vertical transition for s-trans 1,3-butadiene using the Becke-Lee-Yang Parr (BLYP) functional. For this system, extrapolating from triplet and ^50:50Bu state energies gives poor results at either the UHF or BLYP levels; spin-annihilated Hartree-Fock theory is similarly unsuccessful.

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