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Molecular packing, crystallinity, and texture of semiconducting polymers areoften critical to performance. Although frame-works exist to quantify theordering, interpretations are often just qualitative, resulting in impreciseand liberal use of terminology. Here, we reemphasize the continuity of thedegree of molecular ordering and advocate that a more nuanced and consistentterminology is used with regards to crystallinity, semicyrstallinity,paracrystallinity, crystallite/aggregate, and related characteristics. We aremotivated in part by our own imprecise and inconsistent use of terminology andthe need to have a primer or tutorial reference to teach new group members. Weshow that a deeper understanding can be achieved by combining grazing-incidencewide-angle X-ray scattering and differential scanning calorimetry. We classifya broad range of representative polymers into four proposed categories based onthe quantitative analysis of molecular order based on the paracrystallinedisorder parameter (g). A small database is presented for over 10representative conjugated and insulating polymers ranging from amorphous tosemicrystalline. Finally, we outline the challenges to rationally designperfect polymer crystals and propose a new molecular design approach thatenvisions conceptual molecular grafting that is akin to strained and unstrainedhetero-epitaxy in classic (compound) semiconductors thin film growth.

Understanding, Quantifying, and Controlling the Molecular Ordering of  Semi-conducting Polymers: From Novices to Experts and Amorphous to Perfect  Crystals