Zangi Ronen, Kaufman Laura J
Department of Chemistry, Columbia University, New York, NY 10027, USA.
Phys Rev E Stat Nonlin Soft Matter Phys. 2007 May;75(5 Pt 1):051501. doi: 10.1103/PhysRevE.75.051501. Epub 2007 May 4.
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.
我们通过分子动力学模拟研究了不同温度下过冷液体中频率依赖的斯托克斯-爱因斯坦(SE)关系的有效性。结果表明,SE关系在对应于β弛豫和α弛豫区域起始的中间频率下成立。在远低于非高斯参数α2最大值对应的频率处,观察到随着温度降低而增大的大偏差。我们认为,过冷液体中SE关系的失效是由于忽略相关运动而低估了扩散系数所致。