Singlet-triplet excitations and long range entanglement in the spin-orbital liquid candidate FeSc2S4

Abstract

Theoretical models of the spin-orbital liquid (SOL) FeSc$_2$S$_4$ have predicted it to be in close proximity to a quantum critical point separating a spin-orbital liquid phase from a long-range ordered magnetic phase. Here, we examine the magnetic excitations of FeSc$_2$S$_4$ through time-domain terahertz spectroscopy under an applied magnetic field. At low temperatures an excitation emerges that we attribute to a singlet-triplet excitation from the SOL ground state. A three-fold splitting of this excitation is observed as a function of applied magnetic field. As singlet-triplet excitations are forbidden in inversion symmetric pure spin systems, our results demonstrate the non-trivial character of the entangled spin-orbital singlet ground state. Using experimentally obtained parameters we compare to existing theoretical models to determine FeSc$_2$S$_4$'s proximity to the quantum critical point. In the context of these models, we estimate that the characteristic length of the singlet correlations to be $\xi/ (\textbf{a}/2) \approx 8.2$ (where $\textbf{a}/2$ is the nearest neighbor lattice constant) which establishes FeSc$_2$S$_4$ as a SOL with long-range entanglement.