Fast Nuclear Spin Read-Out in Single Molecule Magnets

Nuclear spins in 4f single-molecule magnets (SMMs) are promising qubits or qudits candidates for quantum information processing due to their relative isolation and reduced susceptibility to environmental disturbances, while their hyperfine coupling to the 4f magnetic moments enable readout and control. So far, the nuclear spin states of individual TbPc2 SMMs have been detected in transport measurements via the spin-cascade effect. Here, we demonstrate a fast, field-sweep-free readout of nuclear spin in individual 163DyPc2 (I = 5/2) and 159TbPc2 (I = 3/2) using millikelvin spin-polarized scanning tunneling microscopy. This fast readout is enabled by the hyperfine interactions, which modifies the statistics of the telegraph noise generated by reversals of the Ln3+ moment, thereby revealing the nuclear spin state. We observe nuclear spin relaxation times T1 in excess of minutes. Furthermore, we drive nuclear spin transitions using a radio-frequency field and detect the resulting nuclear magnetic resonance directly in the tunneling current. Thus our approach enables fast access to long-lived nuclear spin states in an individual molecule