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Single-molecule magnets (SMMs) are promising elements for quantuminformatics. In the presence of strong magnetic anisotropy, they exhibitmagnetization blocking - a magnetic memory effect at the level of a singlemolecule. Recent studies have shown that the SMM performance scales with theheight of magnetization blocking barrier. By employing molecular engineeringthis can be significantly modified, remaining independent from other externalfactors such as magnetic field. Taking advantage of hyperfine coupling ofelectronic and nuclear spins further enhances their functionality, however, apoor understanding of relaxation mechanisms in such SMMs limits theexploitation of nuclear-spin molecular qubits. Here we report the openingdiscovery of field-dependent oscillation of the magnetization blocking barrierin a new holmium metallacrown magnet driven by the switch of relaxationmechanisms involving hyperfine interaction. Single-crystal magnetic hysteresismeasurements combined with first-principles calculations reveal an activatedtemperature dependence of magnetic relaxation dominated either by incoherentquantum tunneling of magnetization at anti-crossing points ofexchange-hyperfine states or by Orbach-like processes at crossing points. Wedemonstrate that these relaxation mechanisms can be consecutively switched onand off by increasing the external field, which paves a way for manipulatingthe magnetization dynamics of SMMs using hyperfine interaction.

Field-induced oscillation of magnetization blocking in holmium metallacrown magnet