Sub-gap optical response across the structural phase transition in van der Waals layered \alpha-RuCl$_3$

TL;DR

This study investigates the optical and structural changes in ta-RuClb3 across a phase transition, revealing unusual hysteresis, electronic excitations, and insights into its low-energy electronic structure related to Kitaev physics.

Contribution

It provides detailed optical and structural analysis of ta-RuClb3's phase transition, highlighting the role of symmetry and uncovering new electronic excitations.

Findings

Two-step hysteresis in phase transition with reflectivity change

Electronic excitation near the transition temperature

Phonon frequencies largely unaffected by symmetry change

Abstract

We report magnetic, thermodynamic, thermal expansion, and on detailed optical experiments on the layered compound $\alpha$-RuCl$_3$ focusing on the THz and sub-gap optical response across the structural phase transition from the monoclinic high-temperature to the rhombohedral low-temperature structure, where the stacking sequence of the molecular layers is changed. This type of phase transition is characteristic for a variety of tri-halides crystallizing in a layered honeycomb-type structure and so far is unique, as the low-temperature phase exhibits the higher symmetry. One motivation is to unravel the microscopic nature of spin-orbital excitations via a study of temperature and symmetry-induced changes. We document a number of highly unusual findings: A characteristic two-step hysteresis of the structural phase transition, accompanied by a dramatic change of the reflectivity. An electronic excitation, which appears in a narrow temperature range just across the structural phase transition, and a complex dielectric loss spectrum in the THz regime, which could indicate remnants of Kitaev physics. Despite significant symmetry changes across the monoclinic to rhombohedral phase transition, phonon eigenfrequencies and the majority of spin-orbital excitations are not strongly influenced. Obviously, the symmetry of the single molecular layers determine the eigenfrequencies of most of these excitations. Finally, from this combined terahertz, far- and mid-infrared study we try to shed some light on the so far unsolved low energy (< 1eV) electronic structure of the ruthenium $4d^5$ electrons in $\alpha$-RuCl$_3$.