Publications Repository - Helmholtz-Zentrum Dresden-Rossendorf
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Multiconfigurational calculations of ground state and excited states of tetravalent uranium complexes
The peculiarities of computational actinide chemistry concerning the ground and excited state require state-of-the-art electronic structure methods. Currently, the most popular one is the CASSCF- method for the inclusion of static correlation in combination with CASPT2 for dynamic correlation and CASSI for spin-orbit coupling. This combination is used for the evaluation of excited state energies and transitions for simulating electronic spectra and comparing with experimental findings. Furthermore, for the evaluation of a proper active space the DMRG method is used for a choice based on objective reasonings. It is found, that the CASSCF+CASPT2+CASSI combination is able to recover experimental values quite well even for a small basis set. However, the DMRG method reveals that the active space could potentially be improved by not only considering the two electrons in the seven 5f-orbitals but also including C-N-pi and corresponding C-N-pi* orbitals.
Keywords: CASSCF; DMRG; electron correlation; actinides; uranium; tetravalent; coordination chemistry
Theory Frontiers in Actinide Sciences, 02.-05.02.2020, Santa Fe, USA
Invited lecture (Conferences)
XIIIth Workshop on Modern Methods in Quantum Chemistry, 02.-05.03.2020, Mariapfarr, Österreich