Microstructural control suppresses thermal activation of electron transport at room temperature in polymer transistors

Alessandro Luzio, Fritz Nübling, Jaime Martin, Daniele Fazzi, Philipp Selter, Eliot Gann, Christopher R. McNeill, Martin Brinkmann, Michael Ryan Hansen, Natalie Stingelin, Michael Sommer () and Mario Caironi ()
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Alessandro Luzio: Istituto Italiano di Tecnologia
Fritz Nübling: Technische Universität Chemnitz, Polymerchemie
Jaime Martin: University of the Basque Country UPV/EHU
Daniele Fazzi: Universität zu Köln
Philipp Selter: Westfälische Wilhelms-Universität
Eliot Gann: Monash Univeristy
Christopher R. McNeill: Monash Univeristy
Martin Brinkmann: Université de Strasbourg
Michael Ryan Hansen: Westfälische Wilhelms-Universität
Natalie Stingelin: Georgia Institute of Technology
Michael Sommer: Technische Universität Chemnitz, Polymerchemie
Mario Caironi: Istituto Italiano di Tecnologia

Nature Communications, 2019, vol. 10, issue 1, 1-13

Abstract: Abstract Recent demonstrations of inverted thermal activation of charge mobility in polymer field-effect transistors have excited the interest in transport regimes not limited by thermal barriers. However, rationalization of the limiting factors to access such regimes is still lacking. An improved understanding in this area is critical for development of new materials, establishing processing guidelines, and broadening of the range of applications. Here we show that precise processing of a diketopyrrolopyrrole-tetrafluorobenzene-based electron transporting copolymer results in single crystal-like and voltage-independent mobility with vanishing activation energy above 280 K. Key factors are uniaxial chain alignment and thermal annealing at temperatures within the melting endotherm of films. Experimental and computational evidences converge toward a picture of electrons being delocalized within crystalline domains of increased size. Residual energy barriers introduced by disordered regions are bypassed in the direction of molecular alignment by a more efficient interconnection of the ordered domains following the annealing process.

Date: 2019
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DOI: 10.1038/s41467-019-11125-9

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