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Chain-level structure of semicrystalline polymers in melt- and solution-grown crystals has been debated over the past several decades. Recently, 13C–13C double quantum (DQ) NMR spectroscopy and spin-dynamics simulation have been applied to trace chain trajectory and packing structure of 13C labeled polymers in melt- and solution-grown crystals. We highlight recent NMR studies for (i) packing structure, (ii) chain trajectory, (iii) conformation of the folded chains, (iv) nucleation mechanisms in the early stage of crystallization, and (v) deformation mechanism at the molecular scale of semicrystalline polymers.

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