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Distinct Molecular Motions in a Switchable Chromophore Dielectric 4-N,N-Dimethylamino-4′-N′-methylstilbazolium Trifluoromethanesulfonate

Authors

  • Zhihua Sun,

    1. Key Laboratory of Optoelectronic Materials, Chemistry and Physics, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, China
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  • Junhua Luo,

    Corresponding author
    1. Key Laboratory of Optoelectronic Materials, Chemistry and Physics, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, China
    • Key Laboratory of Optoelectronic Materials, Chemistry and Physics, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, China.
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  • Tianliang Chen,

    1. Key Laboratory of Optoelectronic Materials, Chemistry and Physics, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, China
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  • Lina Li,

    1. Key Laboratory of Optoelectronic Materials, Chemistry and Physics, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, China
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  • Ren-Gen Xiong,

    1. Ordered Matter Science Research Center, Southeast University, Nanjing 210096, China
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  • Ming-Liang Tong,

    1. State Key Laboratory of Optoelectronic, Materials and Technologies, School of Chemistry and Chemical Engineering, Sun Yat-Sen University, Guangzhou 510275, China
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  • Maochun Hong

    1. Key Laboratory of Optoelectronic Materials, Chemistry and Physics, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, China
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Abstract

Molecular motion associated with rotational and orientational phase transitions is one of the prominent structural strategies for assembling the functional materials such as artificial motors and tunable molecular dielectrics. Here, a new organic chromophore molecule, 4-N,N-dimethylamino-4′-N′-methylstilbazolium trifluoromethanesulfonate (complex 1), which undergoes an exceptional order-disorder phase transition at 322 K, is successfully synthesized. The single crystal X-ray diffraction analysis, thermal analysis, and dielectric measurements are used to characterize its dielectric dynamic behaviors. The results reveal that 1 behaves as a molecular rotator with the obviously distorted bipyramidal geometry of trifluoromethanesulfonate anions. In addition to its disorderings, two very distinct motions of the anionic moieties are confirmed, namely the “earth rotation” of partial units and the “earth revolution” of the whole molecule. Such unique molecular motions are found to be mainly responsible for the order–disorder phase transition together with the abrupt dielectric anomaly and anisotropy. The charge-transfer cationic parts enhance the molecular motions behaving as the stator and give rise to its excellent third-order nonlinearities. The concept may allow for the remote control of molecular events to explore functional materials in organic chromophores.

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