journal article·2025-12-12Open access

Universal Soft Coulomb Gap Governs Thermoelectric Performance in Doped Conjugated Polymers

Yuqian Liu, Xiaoran Wei, Dorothea Scheunemann, Maojie Zhang, Wanlu Zhang, Martijn Kemerink, Guangzheng Zuo

ACS Energy Letters· Volume 10· Issue 12

Abstract

The power factor (PF) in doped conjugated polymers is fundamentally constrained by a trade-off between electrical conductivity and the Seebeck coefficient, yet the underlying universal limit remains unclear. Here, we identify a soft Coulomb gap near the Fermi level as the intrinsic origin of this limit, arising from long-range Coulomb repulsion among localized carriers. Combining systematic experiments and kinetic Monte Carlo simulations across chemically diverse materials, we consistently show that the maximum PF coincides with a distinct transition from Mott to Efros–Shklovskii variable-range hopping, marking the onset of gap formation accompanied by Seebeck coefficient suppression. By increasing the dielectric constant or promoting charge delocalization, the soft gap can be effectively suppressed, shifting the optimal doping range and enhancing performance. These findings establish a unifying physical framework and actionable design rules for overcoming the PF limit, with broad implications for the design of high-performance thermoelectric and other doped organic electronic materials
Source: openalex_inverted_index · Quality: baseline

Research context

OpenAlex topics: Organic Electronics and Photovoltaics · Advanced Thermoelectric Materials and Devices · Conducting polymers and applications

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Institute for Electric Light Sources, College of Intelligent Robotics and Advanced Manufacturing

Fudan University

Institute for Molecular Systems Engineering and Advanced Materials

Heidelberg University

National Engineering Research Center for Colloidal Materials, Key Laboratory of Special Functional Aggregated Materials, Ministry of Education, School of Chemistry and Chemical Engineering

Shandong University

Funding

Carl-Zeiss-Stiftung · H2020 Marie Sklodowska-Curie Actions · Science and Technology Commission of Shanghai Municipality

References (42)

Show source-provided references
1. 10.1039/C6CS00149A10.1039/C6CS00149A ↗
2. 10.1021/acs.macromol.9b0245310.1021/acs.macromol.9b02453 ↗
3. 10.1146/annurev-matsci-082219-02471610.1146/annurev-matsci-082219-024716 ↗
4. 10.1016/j.pmatsci.2021.10084010.1016/j.pmatsci.2021.100840 ↗
5. 10.1002/adfm.20221077010.1002/adfm.202210770 ↗
6. 10.1016/j.progpolymsci.2022.10154810.1016/j.progpolymsci.2022.101548 ↗
7. 10.1038/s41586-024-07724-210.1038/s41586-024-07724-2 ↗
8. 10.1557/s43578-024-01321-910.1557/s43578-024-01321-9 ↗
9. 10.1002/adma.20170306310.1002/adma.201703063 ↗
10. 10.1002/aelm.20190094510.1002/aelm.201900945 ↗
11. 10.1002/adma.20220821510.1002/adma.202208215 ↗
12. 10.1002/adma.20240439710.1002/adma.202404397 ↗
13. 10.1126/sciadv.aay806510.1126/sciadv.aay8065 ↗
14. 10.1002/adfm.20200690010.1002/adfm.202006900 ↗
15. 10.1002/aenm.20140107210.1002/aenm.201401072 ↗
16. 10.1021/acs.jpcc.3c0719710.1021/acs.jpcc.3c07197 ↗
17. 10.1103/PhysRevB.96.24120210.1103/PhysRevB.96.241202 ↗
18. 10.1016/j.joule.2025.10214010.1016/j.joule.2025.102140 ↗
19. 10.1002/advs.20240938210.1002/advs.202409382 ↗
20. 10.1103/PhysRevB.82.11545410.1103/PhysRevB.82.115454 ↗
21. 10.1021/acsami.0c1549010.1021/acsami.0c15490 ↗
22. 10.1002/adfm.20170328010.1002/adfm.201703280 ↗
23. 10.1063/1.501690810.1063/1.5016908 ↗
24. 10.1002/adma.20170093010.1002/adma.201700930 ↗
25. 10.1021/jacs.7b0530010.1021/jacs.7b05300 ↗
26. 10.1021/ma402040610.1021/ma4020406 ↗
27. 10.1002/adfm.20230915610.1002/adfm.202309156 ↗
28. 10.1021/ja305188r10.1021/ja305188r ↗
29. 10.1039/D0TC01047B10.1039/D0TC01047B ↗
30. 10.1038/srep4470410.1038/srep44704 ↗
31. 10.1002/adma.20220821510.1002/adma.202208215 ↗
32. 10.1002/adfm.20221282510.1002/adfm.202212825 ↗
33. 10.1039/D4TC01568A10.1039/D4TC01568A ↗
34. 10.1002/adfm.20220207510.1002/adfm.202202075 ↗
35. 10.1002/adma.20210298810.1002/adma.202102988 ↗
36. 10.1021/acs.jpcc.4c0557710.1021/acs.jpcc.4c05577 ↗
37. 10.1088/0022-3719/8/4/00310.1088/0022-3719/8/4/003 ↗
38. 10.1063/10.003434310.1063/10.0034343 ↗
39. 10.1103/PhysRevB.93.23520310.1103/PhysRevB.93.235203 ↗
40. 10.1021/acsami.8b0012210.1021/acsami.8b00122 ↗
41. 10.1002/adma.20231130310.1002/adma.202311303 ↗
42. 10.1103/PhysRevLett.131.24810110.1103/PhysRevLett.131.248101 ↗