Abstract
Understanding how dynamic properties depend on the structure and thermodynamics in liquids is a long-standing open problem in condensed matter physics. A very simple approach is based on the Dzugutov contribution developed on model fluids in which a universal (i.e. species-independent) connection relates the pair excess entropy of a liquid to its reduced diffusion coefficient. However its application to “real” liquids still remains uncertain due to the ability of a hard sphere (HS) reference fluid used in reducing parameters to describe complex interactions that occur in these liquids. Here we use ab initio molecular dynamics simulations to calculate both structural and dynamic properties at different temperatures for a wide series of liquid metals including Al, Au, Cu, Li, Ni, Ta, Ti, Zn as well as liquid Si and B. From this analysis, we demonstrate that the Dzugutov scheme can be applied successfully if a self-consistent method to determine the packing fraction of the hard sphere reference fluid is used as well as the Carnahan-Starling approach to express the excess entropy.
Highlights
Understanding how dynamic properties depend on the structure and thermodynamics in liquids is a long-standing open problem in condensed matter physics
We propose to discuss the validity of the Dzugutov scheme when applied to real liquids by computing the diffusivities, radial distribution functions and excess entropies for various liquid metals, namely Al, Au, Cu, Li, Ni, Ta, Ti, Zn, using ab initio molecular dynamics (AIMD) simulations
We have checked for each element and for one temperature the consistency of the values of D obtained from both routes
Summary
Understanding how dynamic properties depend on the structure and thermodynamics in liquids is a long-standing open problem in condensed matter physics. Theoretical developments of the liquid state dynamics have shown that dynamic properties can be determined from the knowledge of the static structure either directly in the framework of renormalized kinetic theories[5,6,7,8,9] and early versions of the mode coupling theory[10,11] (MCT) or through thermodynamic quantities like entropy in the Adam-Gibbs theory[12] This line of thinking has been subsequently explored in several computational and experimental studies[13,14,15,16,17,18,19]. Collision frequency term developed for hard spheres cannot capture correctly the local atomic structure of this element
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