Frequency-dependent Stokes-Einstein relation in supercooled liquids.
We investigate by molecular dynamics simulations the validity of the frequency-dependent Stokes-Einstein (SE) relation in supercooled liquids at different temperatures. The results indicate that the SE relation holds at intermediate frequencies that correspond to the beta -relaxation and the onset of the alpha -relaxation regimes. Large deviations, which increase as the temperature decreases, are observed at frequencies well below the frequency at which the non-Gaussian parameter alpha2 is maximum. We argue that the breakdown of the SE relation in supercooled liquids arises from underestimation of the diffusion coefficient due to neglect of correlated motions.
Department of Chemistry, Columbia University, New York, NY 10027, USA.
Ronen
R
Zangi
Laura J
LJ
Kaufman