Xu, Kai ORCID: 0000-0002-4653-7853, Ruoko, Tero-Petri, Shokrani, Morteza, Scheunemann, Dorothea ORCID: 0000-0001-9458-7022, Abdalla, Hassan, Sun, Hengda, Yang, Chi-Yuan, Puttisong, Yuttapoom, Kolhe, Nagesh B., Figueroa, Jose Silvestre Mendoza, Pedersen, Jonas O., Ederth, Thomas, Chen, Weimin M., Berggren, Magnus ORCID: 0000-0001-5154-0291, Jenekhe, Samson A., Fazzi, Daniele ORCID: 0000-0002-8515-4214, Kemerink, Martijn and Fabiano, Simone ORCID: 0000-0001-7016-6514 (2022). On the Origin of Seebeck Coefficient Inversion in Highly Doped Conducting Polymers. Adv. Funct. Mater., 32 (20). WEINHEIM: WILEY-V C H VERLAG GMBH. ISSN 1616-3028

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Abstract

A common way of determining the majority charge carriers of pristine and doped semiconducting polymers is to measure the sign of the Seebeck coefficient. However, a polarity change of the Seebeck coefficient has recently been observed to occur in highly doped polymers. Here, it is shown that the Seebeck coefficient inversion is the result of the density of states filling and opening of a hard Coulomb gap around the Fermi energy at high doping levels. Electrochemical n-doping is used to induce high carrier density (>1 charge/monomer) in the model system poly(benzimidazobenzophenanthroline) (BBL). By combining conductivity and Seebeck coefficient measurements with in situ electron paramagnetic resonance, UV-vis-NIR, Raman spectroelectrochemistry, density functional theory calculations, and kinetic Monte Carlo simulations, the formation of multiply charged species and the opening of a hard Coulomb gap in the density of states, which is responsible for the Seebeck coefficient inversion and drop in electrical conductivity, are uncovered. The findings provide a simple picture that clarifies the roles of energetic disorder and Coulomb interactions in highly doped polymers and have implications for the molecular design of next-generation conjugated polymers.

Item Type: Journal Article
Creators:
CreatorsEmailORCIDORCID Put Code
Xu, KaiUNSPECIFIEDorcid.org/0000-0002-4653-7853UNSPECIFIED
Ruoko, Tero-PetriUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Shokrani, MortezaUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Scheunemann, DorotheaUNSPECIFIEDorcid.org/0000-0001-9458-7022UNSPECIFIED
Abdalla, HassanUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Sun, HengdaUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Yang, Chi-YuanUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Puttisong, YuttapoomUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Kolhe, Nagesh B.UNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Figueroa, Jose Silvestre MendozaUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Pedersen, Jonas O.UNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Ederth, ThomasUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Chen, Weimin M.UNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Berggren, MagnusUNSPECIFIEDorcid.org/0000-0001-5154-0291UNSPECIFIED
Jenekhe, Samson A.UNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Fazzi, DanieleUNSPECIFIEDorcid.org/0000-0002-8515-4214UNSPECIFIED
Kemerink, MartijnUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Fabiano, SimoneUNSPECIFIEDorcid.org/0000-0001-7016-6514UNSPECIFIED
URN: urn:nbn:de:hbz:38-690804
DOI: 10.1002/adfm.202112276
Journal or Publication Title: Adv. Funct. Mater.
Volume: 32
Number: 20
Date: 2022
Publisher: WILEY-V C H VERLAG GMBH
Place of Publication: WEINHEIM
ISSN: 1616-3028
Language: English
Faculty: Unspecified
Divisions: Unspecified
Subjects: no entry
Uncontrolled Keywords:
KeywordsLanguage
DESIGNMultiple languages
Chemistry, Multidisciplinary; Chemistry, Physical; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied; Physics, Condensed MatterMultiple languages
URI: http://kups.ub.uni-koeln.de/id/eprint/69080

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