Anomalous frequency and intensity scaling of collective and local modes in a coupled spin tetrahedron system

Abstract

We report on the magnetic excitation spectrum of the coupled spin tetrahedral system Cu$_{2}$Te$_{2}$O$_{5}$Cl$_{2}$ using Raman scattering on single crystals. The transition to an ordered state at T$_{N}^{Cl}$=18.2 K evidenced from thermodynamic data leads to the evolution of distinct low-energy magnetic excitations superimposed by a broad maximum. These modes are ascribed to magnons with different degree of localization and a two-magnon continuum. Two of the modes develop a substantial energy shift with decreasing temperature similar to the order parameter of other Neel ordered systems. The other two modes show only a negligible temperature dependence and dissolve above the ordering temperature in a continuum of excitations at finite energies. These observations point to a delicate interplay of magnetic inter- and intra-tetrahedra degrees of freedom and an importance of singlet fluctuations in describing a spin dynamics.