Anisotropic scattering continuum induced by crystal symmetry reduction in atomically thin α–RuCl3

Abstract

Kitaev quantum spin liquids described by the Kitaev model represent an exotic state of matter with long-range entangled spins and topological order, which hold promise for quantum computation. $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{RuCl}}_{3}$, a material with van der Waals layered structure, is shown to be proximate to such a state recently. Here we report Raman spectroscopy of atomically thin $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{RuCl}}_{3}$. New phonon modes emerge at low temperature, signifying a phase transition to a crystal structure with lowered symmetry. The Fano line shape of two low-energy phonon modes and the magnetic scattering continuum in bulk $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{RuCl}}_{3}$, which evidence fractionalized Majorana fermions of the proximate quantum spin liquid, persist to the trilayer. Polarization-dependent measurements reveal increased anisotropy of the Kitaev exchange constants when approaching the two-dimensional limit. Our results demonstrate an intimate relation between the crystal structure and the symmetry of the proximate quantum spin liquid ground state.