Optical conductivity spectra of the rattling phonons and charge carriers in type-VIII clathrate BaGaSn
Abstract: We have investigated optical conductivity spectra of - and -type BaGa Sn (-BGS) with type-VIII clathrate structure, at temperatures from 296\,K down to 6\,K with a terahertz time-domain spectrometer (0.2\,-\,2.5\,THz). The continuous spectra contributed from charge carriers are dispersive in this frequency range and also temperature- and carrier type-dependent. The Drude-Smith model taking multiple-scatterings of charge carriers into account well reproduces those data. The relaxation rate of the -type carriers decreases more sharply than that in the -type material, suggesting that a stronger electron-phonon interaction may exist in the -type than in the -type. On the other hand, the localized infrared-active modes observed at 1.3\,THz and 1.7\,THz, identified as the rattling phonons of the Ba ion's quasi-on-center vibrations, become soft and broad significantly with decreasing temperature as well as observed in type-I BGS and BGG (BaGaGe) clathrates. The softening in the -type is smaller by about 30% than in the -type, whereas the linewidth brodening is almost the same independently on the carrier type. The difference in the softening is discussed with a scenario where the interaction of rattling phonons with carriers can modify the anharmonic potential of the guest ions. The anomalous broadening at low temepratures is also discussed by the impurity-scattering model presented for a rattling-phonon system strongly hybridized with acoustic cage phonons.
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