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On the Origin of Seebeck Coefficient Inversion in Highly Doped Conducting Polymers
Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. Yanshan Univ, Peoples R China.
Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. Tampere Univ, Finland.ORCID iD: 0000-0003-3091-1051
Heidelberg Univ, Germany.
Heidelberg Univ, Germany.
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2022 (English)In: Advanced Functional Materials, ISSN 1616-301X, E-ISSN 1616-3028, Vol. 32, no 20, article id 2112276Article in journal (Refereed) Published
Abstract [en]

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.

Place, publisher, year, edition, pages
Wiley-V C H Verlag GMBH , 2022. Vol. 32, no 20, article id 2112276
Keywords [en]
conducting polymers; organic electrochemical transistor; Seebeck coefficient; thermoelectric application
National Category
Condensed Matter Physics
Identifiers
URN: urn:nbn:se:liu:diva-182954DOI: 10.1002/adfm.202112276ISI: 000751371400001OAI: oai:DiVA.org:liu-182954DiVA, id: diva2:1638277
Note

Funding Agencies|Swedish Research CouncilSwedish Research CouncilEuropean Commission [2020-03243]; Olle Engkvists Stiftelse [204-0256]; European CommissionEuropean CommissionEuropean Commission Joint Research Centre [GA-955837, GA-799477]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University [SFO-Mat-LiU 2009-00971]; Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germanys Excellence Strategy via the Excellence Cluster 3D Matter Made to OrderGerman Research Foundation (DFG) [EXC-2082/1-390761711]; Carl Zeiss Foundation; Deutsche ForschungsgemeinschaftGerman Research Foundation (DFG) [FA 1502/1-1]; National Natural Science Foundation of ChinaNational Natural Science Foundation of China (NSFC) [52173156]; Swedish Foundation for Strategic ResearchSwedish Foundation for Strategic Research [ITM17-0316]

Available from: 2022-02-16 Created: 2022-02-16 Last updated: 2023-12-28Bibliographically approved

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Ruoko, Tero-PetriAbdalla, HassanSun, HengdaYang, ChiyuanPuttisong, YuttapoomEderth, ThomasChen, WeiminBerggren, MagnusKemerink, MartijnFabiano, Simone

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Xu, KaiRuoko, Tero-PetriAbdalla, HassanSun, HengdaYang, ChiyuanPuttisong, YuttapoomMendoza Figueroa, SilvestreOshaug Pedersen, JonasEderth, ThomasChen, WeiminBerggren, MagnusKemerink, MartijnFabiano, Simone
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