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Establishing Self-Dopant Design Principles from Structure–Function Relationships in Self-n-Doped Perylene Diimide Organic Semiconductors

Powell, D; Zhang, X; Nwachukwu, CI; Miller, EJ; Hansen, KR; Flannery, L; Ogle, J; ... Whittaker-Brooks, L; + view all (2022) Establishing Self-Dopant Design Principles from Structure–Function Relationships in Self-n-Doped Perylene Diimide Organic Semiconductors. Advanced Materials , 34 (42) , Article 2204656. 10.1002/adma.202204656. Green open access

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Abstract

Self-doping is a particular doping method that has been applied to a wide range of organic semiconductors. However, there is a lack of understanding regarding the relationship between dopant structure and function. A structurally diverse series of self-n-doped perylene diimides (PDIs) is investigated to study the impact of steric encumbrance, counterion selection, and dopant/PDI tether distance on functional parameters such as doping, stability, morphology, and charge-carrier mobility. The studies show that self-n-doping is best enabled by the use of sterically encumbered ammoniums with short tethers and Lewis basic counterions. Additionally, water is found to inhibit doping, which concludes that thermal degradation is merely a phenomenological feature of certain dopants, and that residual solvent evaporation is the primary driver of thermally activated doping. In situ grazing-incidence wide-angle X-ray scattering studies show that sample annealing increases the π–π stacking distance and shrinks grain boundaries for improved long-range ordering. These features are then correlated to contactless carrier-mobility measurements with time-resolved microwave conductivity before and after thermal annealing. The collective relationships between structural features and functionality are finally used to establish explicit self-n-dopant design principles for the future design of materials with improved functionality.

Type: Article
Title: Establishing Self-Dopant Design Principles from Structure–Function Relationships in Self-n-Doped Perylene Diimide Organic Semiconductors
Open access status: An open access version is available from UCL Discovery
DOI: 10.1002/adma.202204656
Publisher version: https://doi.org/10.1002/adma.202204656
Language: English
Additional information: This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions.
UCL classification: UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Electronic and Electrical Eng
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL
URI: https://discovery.ucl.ac.uk/id/eprint/10157830
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