Different metrics for connecting mobility and glassiness in thin films

Abstract

Data continue to accrue indicating that experimental techniques may differ in their sensitivity to mobility and glassiness. In this work the Limited Mobility (LM) kinetic model is used to show that two metrics for tracking sample mobility yield quantitatively different results for the glass transition and mobile layer thickness in systems where free surfaces are present. Both LM metrics track the fraction of material that embodies mobile free volume; in one it is relative to that portion of the sample containing any kind (mobile and dormant) of free volume, and in the other it is relative to the overall sample. Without any kind of optimization, use of the latter metric leads to semi-quantitative agreement with experimental film results, both for the mobile layer thickness and the dependence of sample glass transition temperature on film thickness. Connecting the LM predictions with experiment also produces a semi-quantitative mapping between LM model length and temperature scales, and those of real systems.