Samuel, JJ and Garudapalli, A and Gangadharappa, C and Mahapatra, SR and Patil, S and Aetukuri, NPB (2022) Charge polarity-dependent ion-insertion asymmetry during electrochemical doping of an ambipolar π-conjugated polymer. In: Nature Communications, 13 (1).
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Abstract
Electrochemical doping is central to a host of important applications such as bio-sensing, neuromorphic computing and charge storage. However, the mechanisms that enable electrochemical dopability and the various parameters that control doping efficiencies are poorly understood. Here, employing complementary electrochemical and spectroelectrochemical measurements, we report a charge-polarity dependent ion insertion asymmetry in a diketopyrrolopyrrole-based ambipolar π-conjugated polymer. We argue that electrostatic interactions are insufficient to fully account for the observed charge-specific ion insertion into the polymer matrix. Using polymer side-chain dependent electrochemical doping studies, we show that electron density donating and accepting tendencies of polymer side-chains sufficiently describe the observed charge-polarity dependent electrochemical doping. Our observations are akin to the solvation of dopant ions by polymer side-chains. We propose that Gutmann donor/acceptor number framework qualifies the ‘solvent-like’ properties of polymer side-chains and provides a rational basis for designing π-conjugated polymers with favorable mixed ionic electronic transport properties.
| Item Type: | Journal Article |
|---|---|
| Publication: | Nature Communications |
| Publisher: | Nature Research |
| Additional Information: | The copyright for this article belongs to the Authors. |
| Keywords: | asymmetry; electrochemical method; electron density; parameter estimation; polymer |
| Department/Centre: | Division of Chemical Sciences > Solid State & Structural Chemistry Unit |
| Date Deposited: | 25 Jan 2023 06:12 |
| Last Modified: | 25 Jan 2023 06:12 |
| URI: | https://eprints.iisc.ac.in/id/eprint/79490 |
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