Cui Linfeng, Gong Yanjun, Cheng Chuanqin, Guo Yongxian, Xiong Wei, Ji Hongwei, Jiang Lang, Zhao Jincai, Che Yanke
Beijing National Laboratory for Molecular Sciences Key Laboratory of Photochemistry Institute of Chemistry Chinese Academy of Sciences University of Chinese Academy of Sciences Beijing 100049 China.
Key Laboratory of Colloid and Interface Chemistry Ministry of Education School of Chemistry and Chemical Engineering Shandong University Jinan 250100 China.
Adv Sci (Weinh). 2021 Jan 4;8(4):2002615. doi: 10.1002/advs.202002615. eCollection 2021 Feb.
Real-time, high signal intensity, and prolonged detection is challenging because of the rarity of fluorophores with both high photostability and luminescence efficiency. In this work, new donor-acceptor (D-A) molecules for overcoming these limitations are reported. A hybridized local and an intramolecular charge-transfer excited state is demonstrated to afford high photoluminescence efficiency of these D-A molecules in solution (≈100%). The twisted molecular structure and bulky alkyl chains effectively suppress - and dipole-dipole interactions, enabling high luminescence efficiency of and in the solid state (≈94% and 100%). Furthermore, two D-A aggregates exhibit high photostability as evidenced by 4% and 8% of the fluorescence decreasing after 6 h of continuous irradiation in air, which is in sharp contrast to ≈95% of fluorescence decreasing in a reference compound. Importantly, with these molecules, ultrasensitive detection of sulfur mustard (SM) with a record limit of 10 ppb and selective detection of SM in complex matrices are achieved.
由于兼具高光稳定性和发光效率的荧光团十分罕见，因此实现实时、高信号强度和长时间检测具有挑战性。在这项工作中，报道了用于克服这些限制的新型供体-受体（D-A）分子。研究表明，杂化局域和分子内电荷转移激发态可使这些D-A分子在溶液中具有高光致发光效率（约100%）。扭曲的分子结构和庞大的烷基链有效抑制了π-π堆积和偶极-偶极相互作用，使得这些D-A分子在固态下具有高发光效率（约94%和100%）。此外，两种D-A聚集体表现出高光稳定性，在空气中连续照射6小时后，荧光分别降低了4%和8%，这与参考化合物中约95%的荧光降低形成鲜明对比。重要的是，使用这些分子，实现了对芥子气（SM）的超灵敏检测，检测限低至10 ppb，并能在复杂基质中对SM进行选择性检测。
