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    Ion-exchange doped polymers at the degenerate limit: what limits conductivity at 100% doping efficiency?

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    Type
    Preprint
    Authors
    Jacobs, Ian E.
    D'Avino, Gabriele
    Lin, Yue
    Lemaur, Vincent
    Huang, Yuxuan
    Ren, Xinglong
    Simatos, Dimitrios
    Wood, William
    Chen, Chen
    Harrelson, Thomas
    Mustafa, Tarig
    O'Keefe, Christopher A.
    Spalek, Leszek
    Tjhe, Dion
    Statz, Martin
    Lai, Lianglun
    Finn, Peter A.
    Neal, William G.
    Strzalka, Joseph
    Nielsen, Christian B.
    Lee, Jin-Kyun
    Barlow, Stephen
    Marder, Seth R.
    McCulloch, Iain cc
    Fratini, Simone
    Beljonne, David
    Sirringhaus, Henning
    KAUST Department
    Chemical Science Program
    KAUST Solar Center (KSC)
    Physical Science and Engineering (PSE) Division
    Date
    2021-01-05
    Permanent link to this record
    http://hdl.handle.net/10754/666841
    
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    Abstract
    Doping of semiconducting polymers has seen a surge in research interest driven by emerging applications in sensing, bioelectronics and thermoelectrics. A recent breakthrough was a doping technique based on ion-exchange, which separates the redox and charge compensation steps of the doping process. The improved microstructural control this process allows enables us for the first time to systematically address a longstanding but still poorly understood question: what limits the electrical conductivity at high doping levels? Is it the formation of charge carrier traps in the Coulomb potentials of the counterions, or is it the structural disorder in the polymer lattice? Here, we apply ion-exchange doping to several classes of high mobility conjugated polymers and identify experimental conditions that achieve near 100% doping efficiency under degenerate conditions with nearly 1 charge per monomer. We demonstrate very high conductivities up to 1200 S/cm in semicrystalline polymer systems, and show that in this regime conductivity is poorly correlated with ionic size, but strongly correlated with paracrystalline disorder. This observation, backed by a detailed electronic structure model that incorporates ion-hole and hole-hole interactions and a carefully parameterized model of disorder, indicates that trapping by dopant ions is negligible, and that maximizing crystalline order is critical to improving conductivity.
    Publisher
    arXiv
    arXiv
    arXiv:2101.01714
    Additional Links
    https://arxiv.org/pdf/2101.01714
    Collections
    Preprints; Physical Science and Engineering (PSE) Division; Chemical Science Program; KAUST Solar Center (KSC)

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