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Intercrystallite molecular connections are widely recognized to tremendously impact the macroscopic properties of semicrystalline polymers. Because it is challenging to directly probe such connections, theoretical frameworks have been developed to quantify their concentrations and predict the mechanical properties that result from these connections. Tie-chain connectivity similarly impacts the electrical properties in semicrystalline conjugated polymers. Yet, its quantitative impact has eluded the community. Here, we assess the Huang-Brown model, a framework commonly used to describe the structural origins of mechanical properties in polyolefins, to quantitatively elucidate the effect of tie chains on the electrical properties of a model conjugated polymer. We found that a critical tie-chain fraction of 10 -3 is needed to support macroscopic charge transport, below which intercrystallite connectivity limits charge transport, and above which intracrystallite disorder is the bottleneck. Extending the Huang-Brown framework to conjugated polymers enables the prediction of macroscopic electrical properties based on experimentally accessible morphological parameters. Our study implicates the importance of long and rigid polymer chains for efficient charge transport over device length scales.

Assessing the Huang–Brown Description of Tie Chains for Charge Transport in Conjugated Polymers