Precision hyperfine spectroscopy of an individual nuclear-spin-9/2
Single-spin magnetic resonance spectroscopy promises to yield structural and chemical information at the level of individual atoms or molecules, in a non-invasive way. Here, we use an Er3+ paramagnetic center in a CaWO4 crystal, detected by microwave photon counting at 10 mK, as a nanoscale magnetic sensor to measure the NMR spectrum of a proximal individual nuclear-spin-9/2 93Nb impurity with Hertz spectral resolution. From these measurements, we determine the 93Nb insertion site, its position relative to the Er3+ , and its complete quadrupolar tensor. We moreover harness the high spectral resolution of our measurements to establish the presence of two previously unobserved terms in the spin Hamiltonian. The first describes a coupling between the Er3+ spin and the 93Nb nuclear quadrupole; it possibly originates from a spin-dependent electrostatic interaction between the two systems. The second is a nuclear hexadecapolar term, and may be caused by the coupling of the electric field third derivative to the 93Nb nuclear hexadecapolar moment.