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Changes in the dynamics of supported polymer films in comparison to bulkmaterials involve a complex convolution of effects, such as substrateinteractions, roughness and compliance, in addition to film thickness. Weconsider molecular dynamics simulations of substrate-supported, coarse-grainedpolymer films where these parameters are tuned separately to determine how eachof these variables influence the molecular dynamics of thin polymer films. Wefind that all these variables significantly influence the film dynamics,leading to a seemingly intractable degree of complexity in describing thesechanges. However, by considering how these constraining variables influencestring-like collective motion within the film, we show that all ourobservations can be understood in a unified and quantitative way. Morespecifically, the string model for glass-forming liquids implies that thechanges in the structural relaxation of these films are governed by the changesin the average length of string-like cooperative motions and this model isconfirmed under all conditions considered in our simulations. Ultimately, thesechanges are parameterized in terms of just the activation enthalpy and entropyfor molecular organization, which have predictable dependences on substrateproperties and film thickness, offering a promising approach for the rationaldesign of film properties.

A Unifying Framework to Quantify the Effects of Substrate Interactions, Stiffness, and Roughness on the Dynamics of Thin Supported Polymer Films