Quantum Coherence between High Spin Superposition States of Single Molecule Magnet Ni₄

Magnetic quantum tunneling in a single molecule magnet (SMM) has been studied in experiments that combine microwave spectroscopy with high sensitivity magnetic measurements. By monitoring spin-state populations in the presence of microwave magnetic fields, the energy splittings between low lying high spin superposition states of SMM Ni$_4$ ($S$ = 4) have been measured. Absorption linewidths give an upper bound on the rate of decoherence. Pulsed microwave experiments provide a direct measure of the spin-lattice relaxation time, which is found to be remarkably long ($\sim$sec) and to increase with the energy splitting.