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Simulation studies based on the embedded crystallite method are used to predict, with no free parameters, complex dynamical behavior for a simple alkali halide defect system, Na+ in KI. Far infrared spectroscopic measurements, including uniaxial stress, confirm the predicted vibrational properties, indicating that this methodology can readily be used for complex and extended defects in ionic crystals.

Vibrational Pocket Modes: Predictions by the Embedded Crystallite Method and Their Experimental Observation