  We have applied ab initio molecular dynamics (MD) simulations to study
metal-metal coupling on the alkali-metal sublattice in the {\beta}-pyrochlore
osmates, AOs2O6 (A = K, Rb, Cs) at 300 K. We find that the alkali-metal atoms
(rattlers) couple to each other more strongly than they couple to the cage
atoms, and that, at 300 K, this coupling is strongest for Cs. We show that this
coupling controls the dominant dynamics in the rattling of these atoms. We
provide preliminary evidence that the rattlers couple to each other primarily
through the T2g mode whereas their coupling to the cage modes occurs through
the T1u mode. Rattler coupling through the T2g mode provides insight into the
trend in spectral broadening from Cs to K. The spectral broadening is inversely
proportional to the strength of the dynamical correlations on the alkali-metal
sublattice which in turn depend on the atomic size of the rattler, decreasing
from Cs to K. Thus, the broadest spectrum exhibited by the K is partly a
consequence of the small size of this rattler which permits a greater range of
motions involving combinations of both correlated and anti-correlated dynamics.
We emphasize that the identification of the somewhat distinct roles of the T1u
and T2g modes in rattler coupling reported in this work is a significant step
towards a complete fundamental mechanism of rattler dynamical coupling in these
osmates. We believe that such a mechanism will have profound implications for a
broad class of cage compounds, including clathrates and skutterudites.
