Electrochemical Doping in Ordered and Disordered Domains of Organic Mixed Ionic-Electronic Conductors.

Cavassin, Priscila; Holzer, Isabelle; Tsokkou, Demetra; Bardagot, Olivier; Réhault, Julien; Banerji, Natalie (2023). Electrochemical Doping in Ordered and Disordered Domains of Organic Mixed Ionic-Electronic Conductors. Advanced materials, 35(35), e2300308. Wiley 10.1002/adma.202300308

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Conjugated polymers are increasingly used as organic mixed ionic-electronic conductors in electrochemical applications for neuromorphic computing, bioelectronics and energy harvesting. The design of efficient electrochemical devices relies on large modulations of the polymer conductivity, fast doping/dedoping kinetics, and high ionic uptake. In this work, structure-property relations are established and control of these parameters by the co-existence of order and disorder in the phase morphology is demonstrated. Using in-situ time-resolved spectroelectrochemistry, resonant Raman and terahertz conductivity measurements, the electrochemical doping in the different morphological domains of poly(3-hexylthiophene) is investigated. The main finding is that bipolarons are found preferentially in disordered polymer regions, where they are formed faster and are thermodynamically more favoured. On the other hand, polarons show a preference for ordered domains, leading to drastically different bipolaron/polaron ratios and doping/dedoping dynamics in the distinct regions. A significant enhancement of the electronic conductivity is evident when bipolarons start forming in the disordered regions, while the presence of bipolarons in the ordered regions is detrimental for transport. This study provides significant advances in the understanding of the impact of morphology on the electrochemical doping of conjugated polymers and the induced increase in conductivity. This article is protected by copyright. All rights reserved.

Item Type:

Journal Article (Original Article)

Division/Institute:

08 Faculty of Science > Department of Chemistry, Biochemistry and Pharmaceutical Sciences (DCBP)

UniBE Contributor:

Cavassin, Priscila, Holzer, Isabelle, Bardagot, Olivier Nicolas Ludovic, Réhault, Julien Emile, Banerji, Natalie

Subjects:

500 Science > 540 Chemistry

ISSN:

1521-4095

Publisher:

Wiley

Language:

English

Submitter:

Pubmed Import

Date Deposited:

24 Apr 2023 12:57

Last Modified:

02 Sep 2023 00:13

Publisher DOI:

10.1002/adma.202300308

PubMed ID:

37086157

Uncontrolled Keywords:

electrochemical doping morphology organic mixed ionic-electronic conductors polaron/bipolaron population dynamics spectroelectrochemistry terahertz conductivity

BORIS DOI:

10.48350/181932

URI:

https://boris.unibe.ch/id/eprint/181932

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