title: Structural control of mixed ionic and electronic transport in conducting polymers.
abstract: Poly(3,4-ethylenedioxythiophene) doped with poly(styrenesulfonate),
  PSS, has been utilized for over two decades as a stable, solution-processable hole conductor. While its hole transport properties have been the subject of intense investigation, recent work has turned to
  PSS as a mixed ionic/electronic conductor in applications including bioelectronics, energy storage and management, and soft robotics. Conducting polymers can efficiently transport both holes and ions when sufficiently hydrated, however, little is known about the role of morphology on mixed conduction. Here, we show that bulk ionic and electronic mobilities are simultaneously affected by processing-induced changes in nano- and meso-scale structure in
  PSS films. We quantify domain composition, and find that domain purification on addition of dispersion co-solvents limits ion mobility, even while electronic conductivity improves. We show that an optimal morphology allows for the balanced ionic and electronic transport that is critical for prototypical mixed conductor devices. These findings may pave the way for the rational design of polymeric materials and processing routes to enhance devices reliant on mixed conduction.
authors.affiliation: Department of Bioelectronics, Ecole Nationale Supérieure des Mines, CMP-EMSE, MOC, Gardanne 13541, France.
authors.forename: Jonathan
authors.identifier: http://orcid.org/0000-0002-0602-6485
authors.initials: J
authors.lastname: Rivnay
authors.affiliation: Department of Bioelectronics, Ecole Nationale Supérieure des Mines, CMP-EMSE, MOC, Gardanne 13541, France.
authors.forename: Sahika
authors.initials: S
authors.lastname: Inal
authors.affiliation: Material Science and Engineering Division, National Institute of Standards and Technology (NIST), Gaithersburg, Maryland 20899, USA.|Department of Physics and Astronomy, Washington State University, Pullman, Washington 99164, USA.
authors.forename: Brian A
authors.initials: BA
authors.lastname: Collins
authors.affiliation: Instituto de Ciencia Molecular, Universidad de Valencia, Paterna 46980, Spain.
authors.forename: Michele
authors.initials: M
authors.lastname: Sessolo
authors.affiliation: Department of Bioelectronics, Ecole Nationale Supérieure des Mines, CMP-EMSE, MOC, Gardanne 13541, France.
authors.forename: Eleni
authors.initials: E
authors.lastname: Stavrinidou
authors.affiliation: Department of Bioelectronics, Ecole Nationale Supérieure des Mines, CMP-EMSE, MOC, Gardanne 13541, France.
authors.forename: Xenofon
authors.initials: X
authors.lastname: Strakosas
authors.affiliation: Stanford Synchrotron Radiation Lightsource (SSRL), SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA.
authors.forename: Christopher
authors.initials: C
authors.lastname: Tassone
authors.affiliation: Material Science and Engineering Division, National Institute of Standards and Technology (NIST), Gaithersburg, Maryland 20899, USA.
authors.forename: Dean M
authors.initials: DM
authors.lastname: Delongchamp
authors.affiliation: Department of Bioelectronics, Ecole Nationale Supérieure des Mines, CMP-EMSE, MOC, Gardanne 13541, France.
authors.forename: George G
authors.initials: GG
authors.lastname: Malliaras