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Spatiotemporal emergence of lamellar branching morphology of polymer spherulite has been investigated theoretically in the framework of a phase field model by coupling a crystal solidification potential pertaining to a nonconserved crystal order parameter with a temperature field generated by latent heat of crystallization. A local free-energy density having an asymmetric double well has been utilized to account for a first-order phase transition such as crystallization. To account for the polymorphous nature of polymer crystallization, the phase field order parameter of crystal at the solidification potential of the double-well local free-energy density is modified to be supercooling dependent. The heat conduction equation, incorporating liberation of latent heat along the nonuniform solid-liquid interface, has led to directional growth of various hierarchical structures including lamella, sheaflike structure, and spherulite. Two-dimensional calculations have been carried out based on experimentally accessible material parameters and experimental conditions for the growth of syndiotactic polypropylene spherulite. The simulations illustrate that, under self-generated thermal field, the initial nucleus is anisotropic having lamellar stacks that transforms to a sheaflike structure and eventually to a lamellar branching morphology with a dual-eye-pocket texture at the core. It appears that the released latent heat is responsible for the lamellar side branching and splaying from the main lamellae. On the same token, the heat build-up seemingly prevents the interface boundaries of neighboring spherulites from over running on each other during impingement, thereby forming the grain boundary. (c) 2005 American Institute of Physics.

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Journal of Chemical Physics





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Copyright 2005 American Institute of Physics. The original published version of this article may be found at