Giant exciton Fano resonance in quasi-one-dimensional Ta$_2$NiSe$_5$

Abstract

We report the complex dielectric function of the quasi-one-dimensional chalcogenide Ta$_2$NiSe$_5$, which exhibits a structural phase transition that has been attributed to exciton condensation below $T_c = 326$ K, and of the isostructural Ta$_2$NiS$_5$ which does not exhibit such a transition. Using spectroscopic ellipsometry, we have detected exciton doublets with pronounced Fano lineshapes in both the compounds. The exciton Fano resonances in Ta$_2$NiSe$_5$ display an order of magnitude higher intensity than those in Ta$_2$NiS$_5$. In conjunction with prior theoretical work by E. Rashba, we attribute this observation to the giant oscillator strength of spatially extended exciton-phonon bound states in Ta$_2$NiSe$_5$. The formation of exciton-phonon complexes in Ta$_2$NiS$_5$ and Ta$_2$NiSe$_5$ is confirmed by the pronounced temperature dependence of sharp interband transitions in the optical spectra, whose peak energies and widths scale with the thermal population of optical phonon modes. The description of the optically excited states in terms of strongly overlapping exciton complexes is in good agreement with the hypothesis of an EI ground state.