CAS Key Laboratory of Separation Science for Analytical Chemistry, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian, 116023, China.
University of Chinese Academy of Sciences, Beijing, 100049, China.
Angew Chem Int Ed Engl. 2023 Jan 9;62(2):e202215215. doi: 10.1002/anie.202215215. Epub 2022 Dec 7.
Synthetic fluorescent protein chromophores have been reported for their singlet state fluorescence properties and applications in bioimaging, but rarely for the triplet state chemistries. Herein, we enabled their photo-sensitizing and photo-crosslinking properties through rational modulations. Extension of molecular conjugation and introduction of heavy atoms promoted the generation of reactive oxygen species. Unlike other photosensitizers, these chromophores selectively photo-crosslinked aggregated proteins and uncovered the interactome profiles. We also exemplified their general applications in chromophore-assisted light inactivation, photodynamic therapy and photo induced polymerization. Theoretical calculation, pathway analysis and transient absorption spectroscopy provided mechanistic insights for this triplet state chemistry. Overall, this work expands the function and application of synthetic fluorescent protein chromophores by enabling their triplet excited state properties.
合成荧光蛋白发色团因其单线态荧光性质及其在生物成像中的应用而被报道，但很少涉及三重态化学。在此，我们通过合理的调节使它们具有光敏化和光交联的特性。分子共轭的扩展和重原子的引入促进了活性氧物质的生成。与其他光敏剂不同，这些发色团选择性地光交联聚集蛋白，并揭示了相互作用组谱。我们还举例说明了它们在发色团辅助光失活、光动力疗法和光诱导聚合中的一般应用。理论计算、途径分析和瞬态吸收光谱为这种三重态化学提供了机制见解。总的来说，这项工作通过使合成荧光蛋白发色团具有三重激发态特性，扩展了它们的功能和应用。
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