Temperature effects on the structure and mechanical properties of vapor deposited a-SiO2

Abstract: Amorphous silica (a-SiO2) exhibits unique thermo-mechanical behaviors that set it apart from other glasses. However, there is still limited understanding of how this mechanical behavior is related to the atomic structure and to the preparation conditions of a-SiO2. Here, we used electron beam (e-beam) physical vapor deposition (PVD) to prepare a series of a-SiO2 films grown at different substrate temperatures and then combined molecular simulations with Positronium Annihilation Lifetime Spectroscopy and nanoindentation experiments to establish relations among processing, structure, and mechanical response of the films. Specifically, we found that increase in the growth temperature leads to increase in the elastic moduli and hardness of the films. The relative porosity in the films also increases while the a-SiO2 network itself becomes denser, resulting in an overall increase in density despite increased porosity. In addition, we found that the a-SiO2 films exhibit the same anomalous temperature dependence of elastic modulus as bulk a-SiO2. However, the rate of increase in the elastic modulus with the measurement temperature was found to depend on the density of the a-SiO2 network and therefore on the growth temperature. Our findings provide new insights into the influence of the atomic network structure on the anomalous thermomechanical behavior of a-SiO2 and in turn guidance to control the mechanical properties of a-SiO2 films.