Fluctuating fractionalized spins in quasi-two-dimensional magnetic V0.85PS3

Abstract

Quantum spin liquid (QSL), a state characterized by exotic low energy fractionalized excitations and statistics, is still elusive experimentally and may be gauged via indirect experimental signatures. A remnant of the QSL phase may reflect in the spin dynamics as well as quanta of lattice vibrations, i.e., phonons, via the strong coupling of phonons with underlying fractionalized excitations. Inelastic light scattering (Raman) studies on ${\mathrm{V}}_{1--x}\mathrm{P}{\mathrm{S}}_{3}$ single crystals evidence the spin fractionalization into Majorana fermions deep into the paramagnetic phase reflected in the emergence of a low frequency quasielastic response, along with a broad magnetic continuum marked by a crossover temperature ${T}^{*}\ensuremath{\sim}200$ K from a pure paramagnetic state to a fractionalized spin regime qualitatively gauged via dynamic Raman susceptibility. We found further evidence of anomalies in the phonons' self-energy parameters, in particular, phonon line broadening and line asymmetry evolution at this crossover temperature, attributed to the decaying of phonons into itinerant Majorana fermions. This anomalous scattering response is thus indicative of fluctuating fractionalized spins suggesting a phase proximate to the quantum spin liquid state in this quasi-two-dimensional magnetic system.