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We demonstrate that nascent polymer crystals (i.e., nuclei) are anisotropicentities, with neither spherical nor cylindrical geometry, in contrast toprevious assumptions. In fact, cylindrical, spherical, and other high symmetrygeometries are thermodynamically unfavorable. Moreover, post-criticaltransitions are necessary to achieve the lamellae that ultimately arise duringthe crystallization of semicrystalline polymers. We also highlight howinaccurate treatments of polymer nucleation can lead to substantial errors(e.g., orders of magnitude discrepancies in predicted nucleation rates). Theseinsights are based on quantitative analysis of over four million crystalclusters from the crystallization of prototypical entangled polyethylene melts.New comprehensive bottom-up models are needed to capture polymer nucleation.

Divining the Shape of Nascent Polymer Crystal Nuclei