Release of free-volume bubbles by cooperative-rearrangement regions during the deposition growth of a colloidal glass

Vapor deposition can directly produce ultrastable glasses which are similar to conventional glasses aged over thousands of years. The highly mobile surface layer is believed to accelerate the ageing process of vapor-deposited glasses, but its microscopic kinetics have not been experimentally observed. Here we study the deposition growth kinetics of a two-dimensional colloidal glass at the single-particle level using video microscopy. We observe that newly deposited particles in the surface layer (depth, d < 14 particles) relax via out-of-cage diffusions of individual particles, while particles in the deeper middle layer (14 < d ≲ 100 particles) relax via activation of cooperative-rearrangement regions. These cooperative-rearrangement regions are much larger, more anisotropic and occur more frequently than cooperative-rearrangement regions in the bulk (d ≳ 100 particles) or after deposition. Cooperative-rearrangement regions move towards the surface and released free-volume bubbles at the surface, while the particles within cooperative-rearrangement regions move towards the bulk, resulting in a more compact bulk glass.