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Sci Adv. 2019 Aug 9;5(8):eaaw7757. doi: 10.1126/sciadv.aaw7757. eCollection 2019 Aug.

Tuning conformation, assembly, and charge transport properties of conjugated polymers by printing flow.

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Department of Chemical and Biomolecular Engineering, University of Illinois at Urbana-Champaign, 600 S. Mathews Ave., Urbana, IL 61801, USA.
Department of Materials Science and Engineering, University of Illinois at Urbana-Champaign, 1304 W. Green St., Urbana, IL 61801, USA.
Laboratory for Chemistry of Novel Materials, University of Mons, Place du Parc, 20, B-7000 Mons, Belgium.
Department of Chemistry, Purdue University, 560 Oval Dr., West Lafayette, IN 47907, USA.
Department of Polymer Science and Engineering, Inha University, 100 Inha-ro, Incheon 402-751, South Korea.
Beckman Institute, Molecular Science and Engineering, University of Illinois at Urbana-Champaign, 405 N. Mathews Ave., Urbana, IL 61801, USA.


Intrachain charge transport is unique to conjugated polymers distinct from inorganic and small molecular semiconductors and is key to achieving high-performance organic electronics. Polymer backbone planarity and thin film morphology sensitively modulate intrachain charge transport. However, simple, generic nonsynthetic approaches for tuning backbone planarity and the ensuing multiscale assembly process do not exist. We first demonstrate that printing flow is capable of planarizing the originally twisted polymer backbone to substantially increase the conjugation length. This conformation change leads to a marked morphological transition from chiral, twinned domains to achiral, highly aligned morphology, hence a fourfold increase in charge carrier mobilities. We found a surprising mechanism that flow extinguishes a lyotropic twist-bend mesophase upon backbone planarization, leading to the observed morphology and electronic structure transitions.

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