Theoretical prediction of closed-shell paramagnetism for scandium and yttrium hydride

Following chemical intuition, one would expect that all closed-shell molecules are diamagnetic. However, it is known that this is not the case for some second-row hydrides with low-lying unoccupied (Formula presented.) orbitals due to an unquenching of the total angular momentum in the presence of an external magnetic field. In this article, the transition-metal hydrides ScH and YH are investigated, assuming a similar unquenching effect involving low-lying unoccupied (Formula presented.) and (Formula presented.) orbitals formed from the metal (Formula presented.) orbitals rather than the (Formula presented.) orbitals. We are comparing results obtained with various quantum-chemical methods (HF, CCSD, CCSD(T), CCSDT) and basis sets. The obtained positive values for the magnetizabilities clearly indicate paramagnetic behavior. Vibrational effects on the magnetizability tensor are also considered, but these effects are small and do not change the overall conclusion that both ScH and YH are further examples for closed-shell paramagnetism.