Tyler J. Quill, Garrett LeCroy, Adam Marks, Sarah A. Hesse, Quentin Thiburce, Iain McCulloch, Christopher J. Tassone, Christopher J. Takacs, Alexander Giovannitti, Alberto Salleo

Charge Carrier Induced Structural Ordering And Disordering in Organic Mixed Ionic Electronic Conductors

  • Mechanical Engineering
  • Mechanics of Materials
  • General Materials Science

AbstractOperational stability underpins the successful application of organic mixed ionic‐electronic conductors (OMIECs) in a wide range of fields, including biosensing, neuromorphic computing, and wearable electronics. In this work, we investigate both the operation and stability of a p‐type OMIEC material of various molecular weights. Electrochemical transistor measurements reveal that device operation is very stable for at least 300 charging/discharging cycles independent of molecular weight, provided the charge density is kept below the threshold where strong charge‐charge interactions become likely. When electrochemically charged to higher charge densities, we observe an increase in device hysteresis and a decrease in conductivity due to a drop in the hole mobility arising from long‐range microstructural disruptions. By employing operando X‐ray scattering techniques, we find two regimes of polaron‐induced structural changes: 1) polaron‐induced structural ordering at low carrier densities, and 2) irreversible structural disordering that disrupts charge transport at high carrier densities, where charge‐charge interactions are significant. These operando measurements also reveal that the transfer curve hysteresis at high carrier densities is accompanied by an analogous structural hysteresis, providing a microstructural basis for such instabilities. This work provides a mechanistic understanding of the structural dynamics and material instabilities of OMIEC materials during device operation.This article is protected by copyright. All rights reserved

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