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Semiconducting Conjugated Coordination Polymer with High Charge Mobility Enabled by "4+2" Phenyl Ligands
- Huang, Xing (author)
-
- Fu, Shuai (author)
- Max Planck Inst Polymer Res, D-55128 Mainz, Germany.
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- Lin, Cong (author)
- Hong Kong Polytech Univ, Dept Mech Engn, Hong Kong, Peoples R China.
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- Max Planck Inst Polymer Res, D-55128 Mainz, Germany Hong Kong Polytech Univ, Dept Mech Engn, Hong Kong, Peoples R China. (creator_code:org_t)
- 2023-01-20
- 2023
- English.
- In: Journal of the American Chemical Society. - : AMER CHEMICAL SOC. - 0002-7863 .- 1520-5126. ; 145:4, s. 2430-2438
- Journal article (peer-reviewed)
Abstract
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- 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.
Subject headings
- NATURVETENSKAP -- Kemi -- Materialkemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Materials Chemistry (hsv//eng)
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- By the author/editor
- Huang, Xing
- Fu, Shuai
- Lin, Cong
- Lu, Yang
- Wang, Mingchao
- Zhang, Peng
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- Huang, Chuanhui
- Li, Zichao
- Liao, Zhongquan
- Zou, Ye
- Li, Jian
- Zhou, Shengqiang
- Helm, Manfred
- St Petkov, Petko
- Heine, Thomas
- Bonn, Mischa
- Wang, Hai I.
- Feng, Xinliang
- Dong, Renhao
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