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Rehybridization of Nitrogen Atom Induced Photoluminescence Enhancement under Pressure Stimulation

机译：在压力刺激下氮原子的再杂交诱导光致发光增强

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摘要

The excited state properties of organic fluorescent materials are crucial for their photoelectronic performance. Here, a study on the highly efficient electrofluorescent material 4-(2-(4'-(diphenylamino)-[1,1'-biphenyl]-4-yl)-1H-phenanthro[9,10-d]imidazol-1-yl) benzonitrile (TBPMCN) is carried out, focusing mainly on its crystal structure and photophysical properties under pressure stimulation. The special triangular-cone (TC) configuration of triphenylamine group in TBPMCN crystal exhibits charge-transfer (CT)-dominated excited state property in TBPMCN, which gives rise to a blue-shifted emission in the crystal. Theoretical calculations prove that the TC conformation is a dynamically metastable state, which is higher in energy than the three-blade-propeller (TBP) configuration. In a further piezochromic experiment, a unique rehybridization-induced emission enhancement phenomenon is found in this crystal, which is essentially different from the aggregation-induced emission enhancement (AIEE) mechanism. It can be assigned to the change of excited state property from a CT-dominated state to a hybridized locally excited and charge-transfer state, as a result of the rehybridization of nitrogen atom upon the increased external pressure. This work provides deep insight into the relationship between molecular structure and excited state properties in crystal by means of the pressure stimulation and further enriches the AIEE mechanism. Additionally, the large red-shifted piezochromic phenomenon of this CT material is stressed.
机译：有机荧光材料的激发态特性对其光电性能至关重要。在这里，对高效电致发光材料4-（2-（4'-（二苯氨基）-[1,1'-联苯] -4-基）-1H-菲并[9,10-d]咪唑-1的研究苯甲腈（TBPMCN）的研究主要集中在压力刺激下的晶体结构和光物理性质。 TBPMCN晶体中三苯胺基团的特殊三角锥（TC）构型在TBPMCN中表现出电荷转移（CT）为主的激发态性质，从而在晶体中引起蓝移发射。理论计算证明，TC构型是动态亚稳态，其能量高于三叶桨（TBP）构型。在进一步的变色实验中，在该晶体中发现了独特的由杂化作用引起的发射增强现象，这与聚集诱导的发射增强（AIEE）机制本质上不同。由于氮原子随着外部压力的增加而重新杂化，它可以归因于激发态性质从CT为主的状态转变为杂化的局部激发和电荷转移的状态。这项工作通过压力刺激提供了对晶体中分子结构与激发态性质之间关系的深入了解，并进一步丰富了AIEE机制。另外，该CT材料的大的红移的压致变色现象被强调。

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  • 来源
    《Advanced Functional Materials》 |2017年第1期|1602276.1-1602276.9|共9页
  • 作者

    Zhang Shitong; Dai Yuxiang; Luo Shengyuan; Gao Yu; Gao Na; Wang Kai; Zou Bo; Yang Bing; Ma Yuguang;

  • 作者单位

    Jilin Univ, Coll Chem, State Key Lab Supramol Struct & Mat, Changchun 130012, Peoples R China;

    Jilin Univ, State Key Lab Superhard Mat, Changchun 130012, Peoples R China;

    Jilin Univ, Coll Chem, State Key Lab Supramol Struct & Mat, Changchun 130012, Peoples R China;

    Jilin Univ, Coll Chem, State Key Lab Supramol Struct & Mat, Changchun 130012, Peoples R China;

    Jilin Univ, Educ Technol Ctr, Changchun 130012, Peoples R China;

    Jilin Univ, State Key Lab Superhard Mat, Changchun 130012, Peoples R China;

    Jilin Univ, State Key Lab Superhard Mat, Changchun 130012, Peoples R China;

    Jilin Univ, Coll Chem, State Key Lab Supramol Struct & Mat, Changchun 130012, Peoples R China;

    South China Univ Technol, State Key Lab Luminescent Mat & Devices, Guangzhou 510640, Guangdong, Peoples R China;

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