In this work we introduce an energy-specific TDHF/TDDFT (ES-TD) approach to selectively calculate absorption spectra above a pre-defined energy threshold while maintaining the orthogonality between excited states and the ground state. The algorithm introduced herein is rigorous because the solutions are exact in the full molecular orbital space. It is based on a simple yet effective idea to bracket high-energy spectra using a Davidson-like iterative algorithm of the spin-unrestricted TDHF/TDDFT implementation. Computational performance and accuracy are compared for Rydberg excited states of an alanine dimer, ligand-to-metal charge transfer transitions in Mn2+-doped ZnO semiconductor nanocrystals and high-energy X-ray absorptions in a set of metal tetrachlorides.

Energy-specific linear response TDHF/TDDFT method   for calculating high-energy excited states

243rd National Meeting (2012)

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