Fluorine dynamics in BaF 2 crystal lattice as an example of complex motion in a simple system

Abstract

Fluorine relaxation profiles for a BaF 2 single crystal collected at several temperatures have been analyzed in terms of essentially different motional models: free rotational and free translational diffusion. The analysis has been performed to critically review the sensitivity of field dependent relaxation studies to mechanisms of molecular motions. The tested motional models do not realistically describe the fluorine dynamics within the crystal lattice. They have been chosen to attempt to answer quite fundamental questions regarding the feasibility of the field dependent nuclear spin relaxation studies to provide unique information on dynamic processes: 1. Is it possible to get information about the motional mechanisms by analyzing relaxation profiles collected in a broad frequency range? 2. To what extent is it possible to reasonably reproduce relaxation profiles in terms of unrealistic motional models? It has been concluded from the analysis that the rotational model leading to a single exponential correlation function explains the experimental data much better than the translational one. Validity regimes of the second order perturbation theory have been discussed in the context of the investigated system and the applied models.