Capturing Structural Snapshots during Photochemical Reactions with Ultrafast Raman Spectroscopy: From Materials Transformation to Biosensor Responses
Capturing Structural Snapshots during Photochemical Reactions with Ultrafast Raman Spectroscopy: From Materials Transformation to Biosensor Responses
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DOI：
10.1021/acs.jpclett.8b00373
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发表时间：
2018-06-21
影响因子：
5.7
通讯作者：
Chen, Cheng
中科院分区：
文献类型：
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作者：
Fang, Chong;Tang, Longteng;Chen, Cheng
化学研究物质的组成、结构、性质和转化。需要对相关过程有机械的理解才能将基础知识转化为实际应用。目前超快拉曼作为一种强大的时间分辨振动技术的发展，特别是飞秒受激拉曼光谱（FSRS），已经揭示了各种光敏系统的结构-能量-函数关系。本视角回顾了近期将光学创新纳入其中的工作，包括将宽带上转换多色阵列 (BUMA) 融入可调谐 FSRS 设置中，并展示了其观察金属形态和光解作用的分辨能力，从而产生高质量的薄膜，以及用于钙离子成像的嵌合蛋白生物传感器的荧光调制。我们讨论了在混合时频域中执行 FSRS 的优点，并提出了通过跟踪低频模式和用特定官能团系统地修改化学结构来描述机制的策略。这些化学键层面的独特见解已开始使光学、材料、能源和生命科学领域的功能分子机器的合理设计和精确控制成为可能。
Chemistry studies the composition, structure, properties, and transformation of matter. A mechanistic understanding of the pertinent processes is required to translate fundamental knowledge into practical applications. The current development of ultrafast Raman as a powerful time-resolved vibrational technique, particularly femtosecond stimulated Raman spectroscopy (FSRS), has shed light on the structure-energy-function relationships of various photosensitive systems. This Perspective reviews recent work incorporating optical innovations, including the broad-band up-converted multicolor array (BUMA) into a tunable FSRS setup, and demonstrates its resolving power to watch metal speciation and photolysis, leading to high-quality thin films, and fluorescence modulation of chimeric protein biosensors for calcium ion imaging. We discuss advantages of performing FSRS in the mixed time-frequency domain and present strategies to delineate mechanisms by tracking low-frequency modes and systematically modifying chemical structures with specific functional groups. These unique insights at the chemical-bond level have started to enable the rational design and precise control of functional molecular machines in optical, materials, energy, and life sciences.