Tailored morphology and highly enhanced phonon transport in polymer fibers: a multiscale computational framework

SC Lin and ZL Cai and Y Wang and LL Zhao and CX Zhai, NPJ COMPUTATIONAL MATERIALS, 5, 126 (2019).

DOI: 10.1038/s41524-019-0264-2

Although tremendous efforts have been devoted to enhance thermal conductivity in polymer fibers, correlation between the thermal-drawing conditions and the resulting chain alignment, crystallinity, and phonon transport properties have remained obscure. Using a carefully trained coarse-grained force field, we systematically interrogate the thermal- drawing conditions of bulk polyethylene samples using large-scale molecular dynamics simulations. An optimal combination of moderate drawing temperature and strain rate is found to achieve highest degrees of chain alignment, crystallinity, and the resulting thermal conductivity. Such combination is rationalized by competing effects in viscoelastic relaxation and condensed to the Deborah number, a predictive metric for the thermal-drawing protocols, showing a delicate balance between stress localizations and chain diffusions. Upon tensile deformation, the thermal conductivity of amorphous polyethylene is enhanced to 80% of the theoretical limit, that is, its pure crystalline counterpart. An effective-medium-theory model, based on the serial- parallel heat conducting nature of semicrystalline polymers, is developed here to predict the impacts from both chain alignment and crystallinity on thermal conductivity. The enhancement in thermal conductivity is mainly attributed to the increases in the intrinsic phonon mean free path and the longitudinal group velocity. This work provides fundamental insights into the polymer thermal-drawing process and establishes a complete process-structure-property relationship for enhanced phonon transport in all-organic electronic devices and efficiency of polymeric heat dissipaters.

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