Yin Xiu, Hu Kuo, Xu Kaiyue, Zhai Chunguang, Dong Jiajun, Fan Xianhong, Yao Mingguang
State Key Laboratory of Superhard Materials, College of Physics, Jilin University, No. 2699 Qianjin Street, Changchun 130012, People 's Republic of China.
State Key Laboratory of Superhard Materials, College of Physics, Jilin University, No. 2699 Qianjin Street, Changchun 130012, People 's Republic of China.
Spectrochim Acta A Mol Biomol Spectrosc. 2022 Dec 15;283:121723. doi: 10.1016/j.saa.2022.121723. Epub 2022 Aug 6.
Studying the stimuli-responsive properties of luminescent materials is important for their applications, while the luminescent materials studied up to now usually exhibit emission quenching and red shift in photoluminescence (PL) energy upon compression. Designing luminescent material with abnormal pressure responses remains challenging. Here, we report the discovery of abnormal luminescent properties of FCO-CzS upon compression. A theoretical study on the excited state decay process has been carried out for FCO-CzS at high pressure by hybrid quantum mechanics/molecular mechanics (QM/MM). A significant emission enhancement and blue shift are observed as pressure increases up to 20 GPa. This is opposite to the pressure response behaviours reported for other luminescent materials. It is further revealed that both the unique molecular configuration and the electronic structure change contribute to the anomalous pressure-responsive emission of FCO-CzS, which reduces the non-radiative rate and increases the radiative rate, respectively. Our study provides a strategy for the design of luminescent materials with desired pressure responses.
研究发光材料的刺激响应特性对其应用至关重要，然而迄今为止所研究的发光材料在压缩时通常会出现光致发光（PL）能量的发射猝灭和红移。设计具有异常压力响应的发光材料仍然具有挑战性。在此，我们报告了FCO-CzS在压缩时异常发光特性的发现。通过混合量子力学/分子力学（QM/MM）对FCO-CzS在高压下的激发态衰变过程进行了理论研究。当压力增加到20 GPa时，观察到显著的发射增强和蓝移。这与其他发光材料报道的压力响应行为相反。进一步揭示，独特的分子构型和电子结构变化分别导致了FCO-CzS的异常压力响应发射，这降低了非辐射速率并增加了辐射速率。我们的研究为设计具有所需压力响应的发光材料提供了一种策略。
