We report magnetic, thermodynamic, thermal expansion, and on detailed optical
experiments on the layered compound α-RuCl3 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 4d5
electrons in α-RuCl3.Comment: 22 pages, 9 figure