Chain-Folding and Molecular-Species Segregation in the Crystallization of Linear High Polymers

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Abstract
For linear high polymers, the assumption that chain ends are excluded from the crystal plus the existence of a reasonable width in the distribution of chain lengths is sufficient to cause a minimum in the free energy‐vs‐crystal thickness curve at temperatures well below the melting point. The predicted crystal thickness is relatively insensitive to crystallite‐surface free energy, but is sensitive to the degree of supercooling and the molecular length distribution. At temperatures lower than a few degrees below the equilibrium mp, there exists a thermodynamic driving force for molecular‐species segregation. Hence according to the theory, crystals which are composed of a variety of molecular species are thermodynamically metastable.

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