Emergent Vibronic Spectral Hierarchy in a Kagome Flat-Band Insulator

Abstract: Electron-phonon coupling is usually understood in terms of electronic quasiparticles interacting with dispersive lattice vibrations. Much less is known about the complementary limit in which the relevant phonon mode is itself localized or weakly dispersive. Here we investigate this regime in the kagome compound Rb$<em>{2}$Ni$</em>{3}$S$<em>{4}$, which undergoes an unconventional insulating transition near $T^{*} \approx$ 260-280~K. Combining polarization-resolved Raman spectroscopy with temperature-dependent x-ray diffraction, scanning tunneling microscopy, and electrical, thermal, and magnetic measurements, we show that the transition involves electronic localization without a conventional structural or magnetic order parameter. Raman spectra reveal a giant Franck-Condon progression associated with a nearly dispersionless 333.7~cm$<sup>{-1}$ phonon, decorated by an equally spaced comb-like fine structure with a characteristic spacing of 40.6~cm$<sup>{-1}$. The comb spacing is insensitive to magnetic field, whereas its spectral weight is strongly field tunable. Rather than treating either hierarchy alone as pure phonon effect, we interpret their nested coexistence as evidence for a strongly coupled electron-vibrational manifold involving a localized lattice coordinate. These results identify dispersionless phonons as an active route to vibronic correlations in solids and suggest that such electron-vibrational self-trapping is closely associated with the insulating phase of Rb$</em>{2}$Ni$<em>{3}$S$</em>{4}$.