And so, while MD has been regularly applied to solid crystalline materials, and NMR is widely used to obtain information (such as activation barriers) from materials exhibiting dynamics, the general question of how to determine the nature of motion of guest molecules moving in a host cavity has not, to our knowledge, been directly addressed. As illustrated schematically in Figure , a typical approach is to fit the NMR data, whether spectral line-shapes or relaxation times, to simple motional models. These models are either assumed or obtained qualitatively from simulation methods. Here we present a new approach to predicting 2 H NMR lineshapes directly from the results of MD simulations, and show that the direct prediction of 2 H spectral and lineshape data provides a more complete physical picture than indirect comparisons involve simplified models.