A molecular dynamics examination of the relationship between self- diffusion and viscosity in liquid metals

YJ Lu and H Cheng and M Chen, JOURNAL OF CHEMICAL PHYSICS, 136, 214505 (2012).

DOI: 10.1063/1.4723683

The self-diffusion coefficients D and the viscosities eta of elemental Ni, Cu, and Ni-Si alloys have been calculated over a wide temperature range by molecular dynamics simulations. For elemental Ni and Cu, Arrhenius-law variations of D and eta with temperature dominate. The temperature dependence of D eta can be approximated by a linear relation, whereas the Stokes-Einstein relation is violated. The calculations of D and eta are extended to the regions close to the crystallization of Ni95Si5, Ni90Si10, and the glass transitions of Ni80Si20 and Ni75Si25. The results show that both D and eta strongly deviate from the Arrhenius law in the vicinity of phase transitions, exhibiting a power-law divergence. We find a decoupling of diffusion and viscous flow just above the crystallization of Ni95Si5 and Ni90Si10. For the two glass-forming alloys, Ni80Si20 and Ni75Si25, the relation D eta = const is obeyed as the glass transition is approached, indicating a dynamic coupling as predicted by the mode-coupling theory. This coupling is enhanced with increasing Si composition and at 25%, Si spans a wide temperature range through the melting point. The decoupling is found to be related to the distribution of local ordered structure in the melts. The power-law governing the growth of solid-like clusters prior to crystallization creates a dynamic heterogeneity responsible for decoupling. (C) 2012 American Institute of Physics. http://dx.doi.org/10.1063/1.4723683

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