Quantum Chemical Characterization of Single Molecule Magnets Based on Uranium

Spivak, M.; Vogiatzis, K. D.; Cramer, C. J.; de Graaf, C.; Gagliardi, L.
J. Phys. Chem. A 2017, 121, 1726 (doi:10.1021/acs.jpca.6b10933).

Multiconfigurational electronic structure theory calculations including spin-orbit coupling effects were performed on four uranium-based single-molecule-magnets. Several quartet and doublet states were computed and the energy gaps between spin-orbit states were then used to determine magnetic susceptibility curves. Trends in experimental magnetic susceptibility curves were well reproduced by the calculations, and key factors affecting performance were identified.