Abstract
Spherulites are the most ubiquitous of polycrystalline microstructure of polymers; they develop under a wide range of conditions by the subsequent branching of crystalline lamella that results in an overall spherical shape. Despite significant efforts over decades, the mechanisms behind branching remain unclear. Molecular dynamics simulations in polyethylene reveal the molecular-level origin of noncrystallographic branching and the initial formation of fibrils. We find that the growth of crystalline lamella by reeling in and folding of polymer chains causes surprisingly large local deformation which, in turn, aligns the chains in the neighboring undercooled liquid. Thus, subsidiary grains nucleate with preferred orientations resulting in fibril growth with branching at small angles, consistent with those observed experimentally.
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