Atomic Transport in Dense, Multi-Component Metallic Liquids

TL;DR

This study investigates atomic transport in dense, multi-component metallic liquids, revealing collective dynamics, slow relaxation processes, and the applicability of mode-coupling theory to describe their behavior near the glass transition.

Contribution

It provides new insights into the atomic transport mechanisms in dense metallic liquids and demonstrates the relevance of mode-coupling theory in describing their dynamics.

Findings

Dense packing with packing fraction above 0.5 in PdNiCuP liquid.

Presence of a fast relaxation process before structural relaxation.

Diffusivities align with tracer measurements and viscosity-based calculations.

Abstract

Pd43Ni10Cu27P0 has been investigated in its equilibrium liquid state with incoherent, inelastic neutron scattering. As compared to simple liquids, liquid PdNiCuP is characterized by a dense packing with a packing fraction above 0.5. The intermediate scattering function exhibits a fast relaxation process that precedes structural relaxation. Structural relaxation obeys a time-temperature superposition that extends over a temperature range of 540K. The mode-coupling theory of the liquid to glass transition (MCT) gives a consistent description of the dynamics which governs the mass transport in liquid PdNiCuP alloys. MCT scaling laws extrapolate to a critical temperature Tc at about 20% below the liquidus temperature. Diffusivities derived from the mean relaxation times compare well with Co diffusivities from recent tracer diffusion measurements and diffsuivities calculated from viscosity via the Stokes-Einstein relation. In contrast to simple metallic liquids, the atomic transport in dense, liquid PdNiCuP is characterized by a drastical slowing down of dynamics on cooling, a q^{-2} dependence of the mean relaxation times at intermediate q and a vanishing isotope effect as a result of a highly collective transport mechanism. At temperatures as high as 2Tc diffusion in liquid PdNiCuP is as fast as in simple liquids at the melting point. However, the difference in the underlying atomic transport mechanism indicates that the diffusion mechanism in liquids is not controlled by the value of the diffusivity but rather by that of the packing fraction.