Spin-lattice Relaxation via Quantum Tunneling in Diluted Crystals of Fe4 Single-molecule Magnets

We investigate the dynamic susceptibility of Fe4 single-molecule magnets with integer spin (S = 5) in the form of pure crystals as well as diluted in crystals of isostructural, but nonmagnetic, Ga4 clusters. Below approximately 1 K, the spin-lattice relaxation becomes dominated by a temperature-independent process. The spin-lattice relaxation time τ measured in this “quantum regime” is 12 orders of magnitude shorter than the characteristic time scale of direct phonon-induced processes but agrees with the relaxation times of pure (i.e.,not assisted by phonons) spin tunneling events. The present results show that the latter phenomenon, despite conserving the energy of the ensemble of electronic and nuclear spins, drives the thermalization of electronic spins at very low temperatures. The spin-lattice relaxation time scales with the concentration of Fe4, thus suggesting that the main effect of dipolar interactions is to block tunneling. The data show therefore no evidence for the contribution of collective phonon emission processes, such as phonon superradiance, to the spin-lattice relaxation.