Polarons in Conjugated Polyelectrolytes: A First‐Principles Perspective

Conjugated polyelectrolytes (CPEs) comprised of conjugated backbones and pendant ionic functionalities are versatile organic semiconductors with myriad optoelectronic applications. Although polarons are dominant charge carriers in conducting CPEs owing to strong electron‐phonon coupling, their prope...

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Bibliographic Details
Published in:Advanced functional materials 2022-12, Vol.32 (52), p.n/a
Main Authors: Wan, Yangyang, Zhang, Xu, Bazan, Guillermo C., Nguyen, Thuc‐Quyen, Lu, Gang
Format: Article
Language:English
Subjects:
conjugated polyelectrolytes
Current carriers
Electronic structure
electrostatic interactions
Energy gap
first‐principles
Materials science
Optoelectronics
Organic semiconductors
Polarons
Polyelectrolytes
Principles
Structural stability
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Summary:Conjugated polyelectrolytes (CPEs) comprised of conjugated backbones and pendant ionic functionalities are versatile organic semiconductors with myriad optoelectronic applications. Although polarons are dominant charge carriers in conducting CPEs owing to strong electron‐phonon coupling, their properties are not well understood, especially from a first‐principles perspective. In this study, a comprehensive study on the stability, structural deformation, electronic structure, and optical absorption of positive (or hole)/negative (or electron) polarons and bi‐polarons in CPEs is conducted. It is explored how these properties depend on the electrostatic interaction between the polarons and ionic functionalities, including alkyl chains, ionic groups, and counterions. It is then examined how the bandgap, polaron binding energy, and optoelectronic structure of CPEs can be tuned by various combinations of the donor and acceptor units in their backbones. Finally, electrochemical stability of CPEs is studied and light is shed on the absence of negative polarons in CPEs. The strategy to improve the electrochemical stability of n‐doped CPEs is also discussed. First‐principles study on the stability, structural deformation, electronic structure, and optical absorption of polarons and bi‐polarons in conjugated polyelectrolytes (CPEs) is carried out, from which the structure‐property relationship of CPEs is established and their electrochemical stability is examined, shedding light on the absence of negative polarons in CPEs. The strategy to improve the stability of n‐doped CPEs is also discussed.
ISSN:1616-301X
1616-3028
DOI:10.1002/adfm.202209394