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Kinetic barriers cause polymers to crystallize incompletely, into nanoscalelamellae interleaved with amorphous regions. As a result, crystalline polymersare full of crystal-melt interfaces, which dominate their physical properties.The longstanding theoretical challenge to understand these interfaces has newrelevance, because of accumulating evidence that polymer crystals oftennucleate via a metastable, partially ordered "rotator" phase. To test this idearequires a theory of the bulk and interfacial free energies of the criticalnucleus. We present a new approach to the crystal-melt interface, whichrepresents the amorphous region as a grafted brush of loops in aself-consistent pressure field. We combine this theory with estimates of bulkfree energy differences, to calculate nucleation barriers and rates via rotatorversus crystal nuclei for polyethylene. We find rotator-phase nucleation isindeed favored throughout the temperature range where nucleation is observed.Our methods can be extended to other polymers.

Polymer crystal–melt interfaces and nucleation in polyethylene