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Non-equilibrium transport in polymer mixed ionic–electronic conductors at ultrahigh charge densities

  • Dionisius H. L. Tjhe,
  • Xinglong Ren,
  • Ian E. Jacobs,
  • Gabriele D’Avino,
  • Tarig B. E. Mustafa,
  • Thomas G. Marsh,
  • Lu Zhang,
  • Yao Fu,
  • Ahmed E. Mansour,
  • Andreas Opitz,
  • Yuxuan Huang,
  • Wenjin Zhu,
  • Ahmet Hamdi Unal,
  • Sebastiaan Hoek,
  • Vincent Lemaur,
  • Claudio Quarti,
  • Qiao He,
  • Jin-Kyun Lee,
  • Iain McCulloch,
  • Martin Heeney,
  • Norbert Koch,
  • Clare P. Grey,
  • David Beljonne,
  • Simone Fratini,
  • Henning Sirringhaus

摘要

Conducting polymers are mixed ionic–electronic conductors that are emerging candidates for neuromorphic computing, bioelectronics and thermoelectrics. However, fundamental aspects of their many-body correlated electron–ion transport physics remain poorly understood. Here we show that in p-type organic electrochemical transistors it is possible to remove all of the electrons from the valence band and even access deeper bands without degradation. By adding a second, field-effect gate electrode, additional electrons or holes can be injected at set doping states. Under conditions where the counterions are unable to equilibrate in response to field-induced changes in the electronic carrier density, we observe surprising, non-equilibrium transport signatures that provide unique insights into the interaction-driven formation of a frozen, soft Coulomb gap in the density of states. Our work identifies new strategies for substantially enhancing the transport properties of conducting polymers by exploiting non-equilibrium states in the coupled system of electronic charges and counterions.