Sodium ion self-diffusion in molten NaBr probed over different length scales

Physical Review. E
F Demmel

Abstract

The single-particle dynamics of sodium ions in molten sodium bromide has been investigated with quasielastic neutron scattering. A detailed and rather extensive data analysis procedure allowed determination of the pure sodium ion dynamics with increasing wave vector. Two different evaluation procedures agree perfectly on the resulting diffusion coefficient of sodium ions on long distances. A simple kinetic theory based on binary collisions of hard spheres is not able to reproduce the sodium diffusion coefficient. The derived reduced linewidth from modeling with a Lorentzian spectral function decreases with increasing wave vector towards the first structure factor maximum. That deviation from the hydrodynamic behavior signals the hindrance of the microscopic diffusion process due to the so-called cage effect when microscopic length scales are probed in a dense fluid. The observed quadratic wave-number-dependent decrease might be evidence for a coupling to density fluctuations as the source of the changes in the diffusion process. The results indicate that in the molten salt NaBr near the melting point the self-diffusion process might be governed by similar processes as already observed in dense metallic liquids.

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Aug 15, 2015·Physical Review. E, Statistical, Nonlinear, and Soft Matter Physics·F DemmelF Formisano

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