Polarization-resolved Raman spectroscopy of α-RuCl3 and evidence of room-temperature two-dimensional magnetic scattering

Polarization-resolved Raman spectroscopy was performed and analyzed from large, high-quality, monodomain single crystal of alpha-RuCl3, a proximate Kitaev quantum spin liquid. Spectra were collected with laser polarizations parallel and perpendicular to the honeycomb plane. Pairs of nearly degenerate phonons were discovered and show either a fourfold or twofold polarization angle dependence in their Raman intensity, thereby providing evidence to definitively assign the bulk crystal point group as C-2h. The low-frequency continuum that is often attributed to scattering from pairs of Majorana fermions was also examined and found to disappear when the laser excitation and scattered photon polarizations were perpendicular to the honeycomb plane. This disappearance, along with the behavior of the phonon spectrum in the same polarization configuration, strongly suggests that the scattering continuum is two-dimensional. We argue that this scattering continuum originates from the Kitaev magnetic interactions that survives up to room temperature, a scale larger than the bare Kitaev exchange energy of approximately 50 K.