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Zokaei, Sepideh ; Kim, Donghyun ; Järsvall, Emmy ; Fenton, Abigail M. ; Weisen, Albree R. ; Hultmark, Sandra ; Nguyen, Phong H. ; Matheson, Amanda M. ; Lund, Anja ; Kroon, Renee ; et al ( , Materials Horizons)Molecular doping of a polythiophene with oligoethylene glycol side chains is found to strongly modulate not only the electrical but also the mechanical properties of the polymer. An oxidation level of up to 18% results in an electrical conductivity of more than 52 S cm −1 and at the same time significantly enhances the elastic modulus from 8 to more than 200 MPa and toughness from 0.5 to 5.1 MJ m −3 . These changes arise because molecular doping strongly influences the glass transition temperature T g and the degree of π-stacking of the polymer, as indicated by both X-ray diffraction and molecular dynamics simulations. Surprisingly, a comparison of doped materials containing mono- or dianions reveals that – for a comparable oxidation level – the presence of multivalent counterions has little effect on the stiffness. Evidently, molecular doping is a powerful tool that can be used for the design of mechanically robust conducting materials, which may find use within the field of flexible and stretchable electronics.more » « less
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Thermal Fluctuations Lead to Cumulative Disorder and Enhance Charge Transport in Conjugated PolymersZhang, Wenlin ; Bombile, Joel H. ; Weisen, Albree R. ; Xie, Renxuan ; Colby, Ralph H. ; Janik, Michael J. ; Milner, Scott T. ; Gomez, Enrique D. ( , Macromolecular Rapid Communications)
Abstract All conjugated polymers examined to date exhibit significant cumulative lattice disorder, although the origin of this disorder remains unclear. Using atomistic molecular dynamics (MD) simulations, the detailed structures for single crystals of a commonly studied conjugated polymer, poly(3‐hexylthiophene‐2,5‐diyl) (P3HT) are obtained. It is shown that thermal fluctuations of thiophene rings lead to cumulative disorder of the lattice with an effective paracrystallinity of about 0.05 in the π–π stacking direction. The thermal‐fluctuation‐induced lattice disorder can in turn limit the apparent coherence length that can be observed in diffraction experiments. Calculating mobilities from simulated crystal structures demonstrates that thermal‐fluctuation‐induced lattice disorder even enhances charge transport in P3HT. The mean inter‐chain charge transfer integral is enhanced with increasing cumulative lattice disorder, which in turn leads to pathways for fast charge transport through crystals.