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Semiconducting Conjugated Coordination Polymer with High Charge Mobility Enabled by "4+2" Phenyl Ligands
Max Planck Inst Polymer Res, D-55128 Mainz, Germany..ORCID iD: 0000-0003-4038-2384
Hong Kong Polytech Univ, Dept Mech Engn, Hong Kong, Peoples R China..
Tech Univ Dresden, Fac Chem & Food Chem, Ctr Adv Elect Dresden cfaed, D-01062 Dresden, Germany..
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2023 (English)In: Journal of the American Chemical Society, ISSN 0002-7863, E-ISSN 1520-5126, Vol. 145, no 4, p. 2430-2438Article in journal (Refereed) Published
Abstract [en]

Electrically conductive coordination polymers and metal-organic frameworks are attractive emerging electroactive materials for (opto-)electronics. However, developing semiconducting coordination polymers with high charge carrier mobility for devices remains a major challenge, urgently requiring the rational design of ligands and topological networks with desired electronic structures. Herein, we demonstrate a strategy for synthesizing high-mobility semiconducting conjugated coordination polymers (c-CPs) utilizing novel conjugated ligands with D2h symmetry, namely, "4 + 2" phenyl ligands. Compared with the conventional phenyl ligands with C6h symmetry, the reduced symmetry of the "4 + 2" ligands leads to anisotropic coordination in the formation of c-CPs. Consequently, we successfully achieve a single-crystalline three-dimensional (3D) c-CP Cu4DHTTB (DHTTB = 2,5-dihydroxy-1,3,4,6-tetrathiolbenzene), containing orthogonal ribbon-like pi-d conjugated chains rather than 2D conjugated layers. DFT calculation suggests that the resulting Cu4DHTTB exhibits a small band gap (similar to 0.2 eV), strongly dispersive energy bands near the Fermi level with a low electron-hole reduced effective mass (similar to 0.2m0*). Furthermore, the four-probe method reveals a semiconducting behavior with a decent conductivity of 0.2 S/cm. Thermopower measurement suggests that it is a p-type semiconductor. Ultrafast terahertz photoconductivity measurements confirm Cu4DHTTB's semiconducting nature and demonstrate the Drude-type transport with high charge carrier mobilities up to 88 +/- 15 cm2 V-1 s-1, outperforming the conductive 3D coordination polymers reported till date. This molecular design strategy for constructing high-mobility semiconducting c-CPs lays the foundation for achieving high-performance c-CP-based (opto-)electronics.

Place, publisher, year, edition, pages
AMER CHEMICAL SOC , 2023. Vol. 145, no 4, p. 2430-2438
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Materials Chemistry
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URN: urn:nbn:se:kth:diva-324461DOI: 10.1021/jacs.2c11511ISI: 000927671300001PubMedID: 36661343Scopus ID: 2-s2.0-85146912753OAI: oai:DiVA.org:kth-324461DiVA, id: diva2:1743451
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QC 20230315

Available from: 2023-03-15 Created: 2023-03-15 Last updated: 2023-06-08Bibliographically approved

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Li, Jian

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