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The two binary clathrates with vacancies (□) Rb8Sn44□2 and Cs8Sn44□2 have been examined using powder inelastic neutron scattering (INS). Rattling energies of Rb and Cs are found to be similar by both experiment and calculations, ℏωCs/ℏωRb|Exp.=0.98(1) and ℏωCs/ℏωRb|Calc.=1.0, despite the significant mass difference: mCs/mRb=1.6, which shows that guest-host interaction is non-negligible for the studied system. For Rb8Sn44□2, a low energy phonon mode is observed at ≈3.5 meV, below the phonon mode which in the literature is attributed to the guest atom. The 3.5 meV mode is interpreted to have significant spectral weight of Sn host atoms based on temperature dependence and comparison with published theoretical phonon calculations. The record of low thermal conductivity of the tin clathrates can be attributed to the host structure dynamics rather than the guest atom rattling.

Guest host interaction and low energy host structure dynamics in tin clathrates