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A growing body of experimental work indicates that physical vapor depositionprovides an effective route for preparation of stable glasses, whose propertiescorrespond in some cases to those expected for glasses that have been aged forthousands of years. In this work, model binary glasses are prepared in aprocess inspired by physical vapor deposition, in which particles aresequentially added to the free surface of a growing film. The resulting glassesare shown to be more stable than those prepared by gradual cooling from theliquid phase. However, it is also shown that the composition of the resultingglass, which is difficult to control in physical vapor deposition simulationsof thin films, plays a significant role on the physical characteristics of thematerial. That composition dependence leads to a re- evaluation of previousresults from simulations of thinner films than those considered here, where theequivalent age of the corresponding glasses was overestimated. The simulationspresented in this work, which correspond to films that are approximately 38molecular diameters thick, also enable analysis of the devitrificationmechanism of vapor-deposited glasses. Consistent with experiments, it is foundthat this mechanism consists of a mobility front that propagates from the freeinterface into the interior of the films. Eliminating surface mobilityeliminates this route of transformation into the supercooled liquid.

Model Vapor-Deposited Glasses: Growth Front and Composition Effects