title: Towards an automated and efficient calculation of resonating vibrational states based on state-averaged multiconfigurational approaches.
abstract: Resonating vibrational states cannot consistently be described by single-reference vibrational self-consistent field methods but request the use of multiconfigurational approaches. Strategies are presented to accelerate vibrational multiconfiguration self-consistent field theory and subsequent multireference configuration interaction calculations in order to allow for routine calculations at this enhanced level of theory. State-averaged vibrational complete active space self-consistent field calculations using mode-specific and state-tailored active spaces were found to be very fast and superior to state-specific calculations or calculations with a uniform active space. Benchmark calculations are presented for trans-diazene and bromoform, which show strong resonances in their vibrational spectra.
authors.affiliation: Institut für Theoretische Chemie, Universität Stuttgart, Pfaffenwaldring 55, 70569 Stuttgart, Germany.
authors.forename: Patrick
authors.initials: P
authors.lastname: Meier
authors.affiliation: Institut für Theoretische Chemie, Universität Stuttgart, Pfaffenwaldring 55, 70569 Stuttgart, Germany.
authors.forename: Dominik
authors.initials: D
authors.lastname: Oschetzki
authors.affiliation: Institut für Theoretische Chemie, Universität Stuttgart, Pfaffenwaldring 55, 70569 Stuttgart, Germany.
authors.forename: Florian
authors.initials: F
authors.lastname: Pfeiffer
authors.affiliation: Institut für Theoretische Chemie, Universität Stuttgart, Pfaffenwaldring 55, 70569 Stuttgart, Germany.
authors.forename: Guntram
authors.initials: G
authors.lastname: Rauhut