Dynamics of ultrathin metal films on amorphous substrates

TL;DR

This paper develops a mathematical model to analyze surface perturbation dynamics of ultrathin metal films on amorphous substrates, highlighting the dominance of liquid phase dewetting over solid state transport during laser-induced thermal cycles.

Contribution

The study integrates existing models to compare solid and liquid phase mass transport, revealing liquid phase dewetting's primary role in surface morphology changes during laser processing.

Findings

Solid state mass transport has negligible effect on surface morphology.

Surface deformations are rapidly quenched during cooling.

Liquid phase instabilities dominate pattern formation.

Abstract

A mathematical model is developed to analyze the growth/decay rate of surface perturbations of an ultrathin metal film on an amorphous substrate (SiO_{2}). The formulation combines the approach of Mullins [J. Appl. Phys. v30, 77, 1959] for bulk substrates, in which curvature-driven mass transport and surface deformation can occur by surface/volume diffusion and evaporation-condensation processes, with that of Spencer et al. [Phys. Rev. Lett. v67, 26, 1991] to describe solid state transport in thin films under epitaxial strain. The model is applied to study the relative rate of solid state mass transport as compared to that of liquid phase dewetting in a thin film subjected to fast a thermal pulse. Specifically, we have recently shown that multiple cycles of nanosecond (ns) pulsed laser melting and resolidification of ultrathin metal films on amorphous substrates can lead to the formation of various types of spatially ordered nanostructures [Phys. Rev. B, v75, 235439 (2007)]. The pattern formation has been attributed to the dewetting of the thin film by a hydrodynamic instability. In such experiments the film is in the solid state during a substantial fraction of each thermal cycle. Results of a linear stability analysis based on the aforementioned model suggest that solid state mass transport has negligible effect on morphology changes of the surface. Hence, surface deformation caused by liquid phase instabilities is rapidly quenched-in during the cooling phase. This deformed state is further evolved by subsequent laser pulses. These results have implications to developing accurate computer simulations of thin film dewetting by energetic beams aimed at the manufacturing of optically active nanoscale materials for applications including information processing, optical devices and solar energy harvesting.