Low-energy excitations in the S=(1/2) molecular nanomagnet K6[V₁₅^IVAs6O42(H2O)]·8H2O from proton NMR and µSR

Abstract

Zero- and longitudinal-field muon-spin-rotation (µSR) and 1H NMR measurements on the S=(1/2) molecular nanomagnet K6[V₁₅^IVAs6O42(H2O)]·8H2O are presented. In LF experiments, the muon asymmetry P(t) was fitted by the sum of three different exponential components with fixed weights. The different muon relaxation rates lambdai (i=1,2,3) and the low-field H=0.23 T 1H NMR spin-lattice relaxation rate 1/T1 show a similar behavior for T>50 K: starting from room temperature they increase as the temperature is decreased. The increase of lambdai and 1/T1 can be attributed to the "condensation" of the system toward the lowest-lying energy levels. The gap Delta~550 K between the first and second S=(3/2) excited states was determined experimentally. For T<2 K, the muon relaxation rates lambdai stay constant, independently of the field value H<=0.15 T. The behavior for T<2 K strongly suggests that, at low T, the spin fluctuations are not thermally driven but rather originate from quasielastic intramolecular or intermolecular magnetic interactions. We suggest that the very-low-temperature relaxation rates could be driven by energy exchanges between two almost degenerate S=(1/2) ground states and/or by quantum effects.