Muon spin relaxation studies of critical fluctuations and diffusive spin dynamics in molecular magnets

Systematic studies of magnetic critical exponents in local moment molecular magnets can be made by combining three different types of μSRμSR measurement; zero-field precession, longitudinal relaxation and the frequency shift in transverse field. Systems have been studied with 1D, 2D and 3D structures, having both simple and non-collinear magnetic interactions and the measurements have included investigation of the effect of chirality on the critical spin fluctuations. In the case of the model S=12 Heisenberg antiferromagnetic 1D chain Heisenberg antiferromagnetic quantum critical fluctuations suppress magnetic ordering and TCNQ radical ion salts can provide some excellent examples of this model. In particular, DEOCC–TCNQF4 behaves as a nearly ideal case with no ordering seen down to 20 mK even though the intrachain exchange interaction is 110 K. In contrast the DMTzNC–TCNQ compound orders at 1.5 K, but still shows evidence for significant residual quantum fluctuations in its ordered state in the form of a large suppression of the magnitude of the ordered part of the magnetic moment. From analysis of the characteristic field dependent muon relaxation behaviour as a function of temperature above the transition, the nature of the spin fluctuations is found to change as the transition is approached, suggesting a crossover either to 2D diffusion or to 1D ballistic motion.