Optical Conductivity Spectral Anomalies in the Off-Center Rattling System β-Ba8Ga16Sn30
PhysRevLett_106_015501.pdf 353 KB
Avila, Marcos A.
We present optical conductivity studies of the type-I clathrate Ba_8Ga_<16>Sn_<30>, using a terahertz time-domain spectrometer (0.3-3.0 THz). The lowest-lying spectral peak at 0.72 THz due to the Ba(2) ion's off-center vibration in the oversized cage shows a drastic and anomalous temperature dependence. Below about 100 K, the single broad peak splits into two subpeaks, and with further lowering of the temperature, the spectral shape of this so-called rattling phonon shows non-Boltzmann broadening to the point that the linewidth becomes comparable to the peak frequency. Whereas the initial splitting can be understood by assuming a multiwell anharmonic potential, the strong linewidth broadening toward low temperature cannot, since the Boltzmann factor generally sharpens the low-temperature spectra. The observed behavior suggests strong interaction between the local anharmonic phonons and other excitations.
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The American Physical Society
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Graduate School of Advanced Sciences of Matter