Crystal-field excitations and vibronic modes in the triangular-lattice spin-liquid candidate TbInO3

Abstract

We study the ground-state properties, the electronic excitations, and lattice dynamics in spin-liquid candidate ${\mathrm{TbInO}}_{3}$. By employing polarization-resolved Raman spectroscopy we define the intermultiplet and intramultiplet excitations, and establish the low-energy crystal-field (CF) level scheme. In particular, we demonstrate that the ground state of the ${\mathrm{Tb}}^{3+}$ ions is a non-Kramers doublet, and relate the enhanced linewidth of the CF modes to the magnetic fluctuations near the spin-liquid ground state. We identify the 38 allowed Raman-active phonon modes at low temperature. Moreover, we observe hybrid vibronic excitations involving coupled CF and low-lying phonon modes, suggesting strong spin-lattice dynamics. We develop a model for vibronic states and obtain the parameters of the bare responses and coupling strength. We further demonstrate that the obtained CF level scheme is consistent with specific-heat data.