NMR relaxation and rattling phonons in type-I Ba8Ga16Sn30 clathrate

Abstract

Atomic motion of guest atoms inside semiconducting clathrate cages is considered an important source for glasslike thermal behavior. 69Ga and 71Ga nuclear magnetic resonance studies on type I Ba8Ga16Sn30 show a clear low-temperature relaxation peak attributed to the influence of Ba rattling dynamics on the framework-atom resonance, with a quadrupolar relaxation mechanism as the leading contribution. Data are analyzed using a two-phonon Raman process, according to a recent theory involving localized anharmonic oscillators. Excellent agreement is obtained using this model, with the parameters corresponding to a uniform array of localized oscillators with very large anharmonicity.