Molecular Magnets for Information and Sensing Applications: Response to Fields and Nuclear Spins*

Recent advances have allowed the experimental realizations of quantum bits and quantum gates by using molecular magnets as active elements, as well as the experimental implementation of quantum algorithms within them. In particular, lanthanide-based molecular magnets are promising for such applications because of strong spin-orbit interaction, compatible molecular geometry to devices, and tunability of coupling between electron and nuclear spins via electric field. So far, there is a lack of ab-initio studies of such coupling and tuning corresponding magnetic properties for lanthanide-based molecular magnets. Nearly degenerate f-orbitals and strongly localized f-electrons suggest importance of calculations beyond density-functional theory. Here we investigate how magnetic properties of monometallic terbium-based molecular magnets are influenced by electric field and coupling to nuclear spin, using multireference quantum chemistry methods including scalar relativistic effects and spin-orbit interaction. We present effects of chemical environment and electric field on such coupling and magnetic anisotropy.