Volume 250, 2024

Single-crystalline oligomer-based conductors modeling the doped poly(3,4-ethylenedioxythiophene) family

Abstract

Conductive polymers with highly conjugated systems, such as the doped poly(3,4-ethylenedioxythiophene) (PEDOT) family, are commonly used in organic electronics. However, their structural inhomogeneity with various chain lengths makes it difficult to control their conductivities and structural details. On the other hand, low-molecular-weight materials have well-defined structures but relatively narrow conjugate areas with a limited range of Coulomb repulsion between carriers (Ueff), which hamper the flexible control of conductivities. To bridge this gap, we developed oligomer-based conductors, which are intermediate materials between polymers and low-molecular-weight materials. Using a library of single-crystal charge-transfer salts of oligo(3,4-ethylenedioxythiophene) (oligoEDOT) analogs that model the doped PEDOT family, we have investigated the structure-determining factors affecting their conductivities, such as counter anion variations, lengths of oligomer donor, and band fillings. Through the screening study, we developed oligoEDOT analogs with tunable room temperature conductivities by several orders of magnitude, including a metallic state above room temperature. In this study, we consistently evaluated the electronic structural insights by first-principles calculations and revealed that Ueff is the dominant factor that determines the relationship between the structures and conductivities. The unique features of oligoEDOT conductor systems with widely variable Ueff can differentiate these systems from strongly electron-correlated systems.

Graphical abstract: Single-crystalline oligomer-based conductors modeling the doped poly(3,4-ethylenedioxythiophene) family

Associated articles

Article information

Article type
Paper
Submitted
10 juil. 2023
Accepted
03 août 2023
First published
14 nov. 2023

Faraday Discuss., 2024,250, 348-360

Single-crystalline oligomer-based conductors modeling the doped poly(3,4-ethylenedioxythiophene) family

T. Fujino, R. Kameyama, K. Onozuka, K. Matsuo, S. Dekura, K. Yoshimi and H. Mori, Faraday Discuss., 2024, 250, 348 DOI: 10.1039/D3FD00134B

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