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Crystallization in Ultra-Thin Polymer Films/ Morphogenesis and Thermodynamical Aspects

J.-U. Sommer and G. Reiter. Thermochimica Acta, 432, 135 (2005)

Abstract

We present a computer model for polymer crystallization in ultra-thin films where chains are considered as dynamical units. In our model chains can change their internal state of order by cooperative motions to improve thermodynamic stability. The interplay between reorganization, enthalpic interactions and the morphology of crystals enables us to explain many properties of growth, morphogenesis and melting of polymer lamellae. We emphasize the relation between the thermodynamic stability of non-equilibrium crystals and morphological features which are beyond the average thickness of the lamellae. In particular, we show that melting of polymers is preceded by reorganization processes and the stability of polymer crystals is not necessarily related to the structure formed at the crystallization point. The simulations allow for the determination of some non-equilibrium properties such as the internal energy and the non-equilibrium heat capacity. We show that multiple-peak melting endotherms, result from morphological transformations. The results of our computer simulations are compared with AFM observations in ultra-thin polyethyleneoxide films.

 

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