Possible Quantum Paraelectric State in Kitaev Spin Liquid Candidate H$_{3}$LiIr$_{2}$O$_{6}$

Abstract

A new quantum spin liquid (QSL) candidate material H$_{3}$LiIr$_{2}$O$_{6}$ was synthesized recently and was found not to show any magnetic order or phase transition down to low temperatures. In this work, we study the quantum dynamics of the hydrogen ions, i.e., protons, in this material by combining first-principles calculations and theoretical analysis. We show that each proton and its adjacent oxygen ions form an electric dipole. The dipole interactions and the proton tunneling are captured by a transverse-field Ising model with a quantum disordered paraelectric ground state. The dipole excitations have an energy gap $\Delta_{\mathrm{d}}\simeq 60$ meV, and can be probed by the infrared optical spectroscopy and the dielectric response. We argue that the electric dipole fluctuations renormalize the magnetic interactions in H$_{3}$LiIr$_{2}$O$_{6}$ and lead to a Kitaev QSL state.