Spin dynamics and spin freezing in the triangular lattice antiferromagnets FeGa2S4 and NiGa2S4

Magnetic susceptibility and muon spin relaxation (muSR) experiments have been carried out on the quasi-2D triangular-lattice spin S = 2 antiferromagnet FeGa2S4. The muSR data indicate a sharp onset of a frozen or nearly-frozen spin state at T* = 31(2) K, twice the spin-glass-like freezing temperature T_f = 16(1) K. The susceptibility becomes field dependent below T*, but no sharp anomaly is observed in any bulk property. A similar transition is observed in muSR data from the spin-1 isomorph NiGa2S4. In both compounds the dynamic muon spin relaxation rate lambda_d(T) above T* agrees well with a calculation of spin-lattice relaxation by Chubukov, Sachdev, and Senthil in the renormalized classical regime of a 2D frustrated quantum antiferromagnet. There is no firm evidence for other mechanisms. At low temperatures lambda_d(T) becomes temperature independent in both compounds, indicating persistence of spin dynamics. Scaling of lambda_d(T) between the two compounds is observed from ~T_f to ~1.5T*. Although the muSR data by themselves cannot exclude a truly static spin component below T*, together with the susceptibility data they are consistent with a slowly-fluctuating "spin gel" regime between T_f and T*. Such a regime and the absence of a divergence in lambda_d(T) at T* are features of two unconventional mechanisms: (1) binding/unbinding of Z_2 vortex excitations, and (2) impurity spins in a nonmagnetic spin-nematic ground state. The absence of a sharp anomaly or history dependence at T* in the susceptibility of FeGa2S4, and the weakness of such phenomena in NiGa2S4, strongly suggest transitions to low-temperature phases with unconventional dynamics.Comment: 13 pages, 6 figures, accepted for publication in Physical Review