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Molecular Origin of Strain-Induced Chain Alignment in PDPP-Based Semiconducting Polymeric Thin Films
Authors:Song Zhang  Amirhadi Alesadi  Gage T Mason  Kai-Lin Chen  Guillaume Freychet  Luke Galuska  Yu-Hsuan Cheng  P Blake J St Onge  Michael U Ocheje  Guorong Ma  Zhiyuan Qian  Sujata Dhakal  Zachary Ahmad  Cheng Wang  Yu-Cheng Chiu  Simon Rondeau-Gagné  Wenjie Xia  Xiaodan Gu
Affiliation:1. School of Polymer Science and Engineering, Center for Optoelectronic Materials and Device, The University of Southern Mississippi, Hattiesburg, MS, 39406 USA;2. Department of Civil and Environmental Engineering, North Dakota State University, Fargo, ND, 58108 USA;3. Department of Chemistry and Biochemistry, University of Windsor, Windsor, ON, N9B3P4 Canada;4. Department of Chemical Engineering, National Taiwan University of Science and Technology, Taipei, 106 Taiwan;5. Brookhaven National Lab, National Synchrotron Light Source II, Upton, NY, 11973 USA;6. Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720 USA
Abstract:Donor–acceptor (D–A) type semiconducting polymers have shown great potential for the application of deformable and stretchable electronics in recent decades. However, due to their heterogeneous structure with rigid backbones and long solubilizing side chains, the fundamental understanding of their molecular picture upon mechanical deformation still lacks investigation. Here, the molecular orientation of diketopyrrolopyrrole (DPP)-based D–A polymer thin films is probed under tensile deformation via both experimental measurements and molecular modeling. The detailed morphological analysis demonstrates highly aligned polymer crystallites upon deformation, while the degree of backbone alignment is limited within the crystalline domain. Besides, the aromatic ring on polymer backbones rotates parallel to the strain direction despite the relatively low overall chain anisotropy. The effect of side-chain length on the DPP chain alignment is observed to be less noticeable. These observations are distinct from traditional linear-chain semicrystalline polymers like polyethylene due to distinct characteristics of backbone/side-chain combination and the crystallographic characteristics in DPP polymers. Furthermore, a stable and isotropic charge carrier mobility is obtained from fabricated organic field-effect transistors. This study deconvolutes the alignment of different components within the thin-film microstructure and highlights that crystallite rotation and chain slippage are the primary deformation mechanisms for semiconducting polymers.
Keywords:chain alignment  coarse-grained molecular dynamics  conjugated polymers  stress–strain  stretchable electronics  tender X-ray
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