Interface Sharpening in Miscible and Isotopic Multilayers: Role of Short-Circuit Diffusion

TL;DR

This study reveals that atomic diffusion at nanoscales can cause interface sharpening in multilayers, even in miscible systems, due to short-circuit diffusion paths, challenging previous assumptions about diffusion behavior.

Contribution

It demonstrates a general phenomenon of interface sharpening during annealing in miscible multilayers, independent of diffusivity asymmetry, using both elemental and isotopic multilayer systems.

Findings

Interface sharpening observed at 423 K in Cu/Ni multilayers.

Isotopic multilayers also show sharpening at 523 K.

Short-circuit diffusion paths like triple junctions are responsible.

Abstract

Atomic diffusion at nanometer length scale may differ significantly from bulk diffusion, and may sometimes even exhibit counterintuitive behavior. In the present work, taking Cu/Ni as a model system, a general phenomenon is reported which results in sharpening of interfaces upon thermal annealing, even in miscible systems. Anomalous x-ray reflectivity from a Cu/Ni multilayer has been used to study the evolution of interfaces with thermal annealing. Annealing at 423 K results in sharpening of interfaces by about 38%. This is the temperature at which no asymmetry exists in the inter-diffusivities of Ni and Cu. Thus, the effect is very general in nature, and is different from the one reported in the literature, which requires a large asymmetry in the diffusivities of the two constituents [Z. Erd\'elyi et al., Science 306, 1913 (2004).]. General nature of the effect is conclusively demonstrated using isotopic multilayers of 57Fe/naturalFe, in which evolution of isotopic interfaces has been observed using nuclear resonance reflectivity. It is found that annealing at suitably low temperature (e.g. 523 K) results in sharpening of the isotopic interfaces. Since chemically it is a single Fe layer, any effect associated with concentration dependent diffusivity can be ruled out. The results can be understood in terms of fast diffusion along short-circuit paths like triple junctions, which results in an effective sharpening of the interfaces at relatively low temperatures.