Recently, quantum logic gates and quantum algorithms have been experimentally realized within some magnetic molecules including single-molecule magnets. For such applications, either molecular electronic levels or nuclear levels can be used for quantum bits and they can be read, operated, or written using magnetic or electric field. In particular, lanthanide-based single-molecule magnets are promising for such applications because of strong spin-orbit interaction, molecular geometry compatible to devices, and tunability of coupling between electron and nuclear spins via external means. Motivated by the recent experimental work, we investigate the nature of hyperfine interactions in trivalent and divalent Tb-based single-molecule magnets with and without an electric field, using multiconfigurational ab-initio methods including spin-orbit coupling. In the absence of an external electric field, we show that trivalent and divalent Tb-based molecules have different types of dominant contributions to the magnetic hyperfine interaction, and that the principal axes of the nuclear quadrupole interaction are not necessarily parallel to those of the magnetic axes. We further examine how the magnetic hyperfine and nuclear quadrupole interactions are influenced by electric field in the Tb-based single-molecule magnets, as a function of the magnitude and direction of electric field. We compare our results with experimental data.

Electric-field control of hyperfine interactions in Tb-based single-molecule magnets for quantum information science

ACS Spring Meeting 2021

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