In-situ TEM observations of abnormal grain growth, coarsening, and substrate de-wetting in nanocrystalline Ag thin films

Abstract

Abnormal grain growth is studied in nanocrystalline sputtered Ag films. Eighty nanometer thick Ag films are DC sputter deposited onto back-etched amorphous silicon nitride membranes. Specimens are annealed in a heating stage in an in-situ TEM for various temperatures and hold times. With the same specimen, we proceed to higher temperatures after the apparent halt of growth for sufficiently long hold times. The grain size distribution of the as-deposited films is bi-modal, with large abnormal grains with 100 nm diameters, embedded in a matrix of smaller grains of 15 nm diameters. Coarsening begins at temperatures of approximately 100°C, and quickly reaches a plateau. The growth process restarts only after sufficient temperature increases, and plateaus at each succeeding temperature. Using a variation of the Mullins–Von Neumann law, the activation energy for the abnormal growth is found to be 0.274 eV, consistent with the value reported for pore formation during electromigration via surface diffusion in Ag. Grain growth appears to stop above temperatures of 350°C, eventually leading to triple junction pore formation at 350°C and de-wetting of the film from the substrate at 600°C. The de-wetting is the high temperature limit of the thermal grooving which cancels the driving force for grain growth at the lower temperatures. TEM images as evidence of this effect are presented, along with observations on the pore formation that support surface diffusion as the mass transport mechanism for grooving, pore fomation, and as the limiting mass transport mechanism for the grain growth.