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.

中文翻译：

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使用超快速拉曼光谱在光化学反应过程中捕获结构快照：从材料转化到生物传感器响应

化学研究物质的组成，结构，性质和转化。需要对相关过程进行机械理解，才能将基础知识转化为实际应用。超快拉曼作为一种功能强大的时间分辨振动技术的最新发展，尤其是飞秒激发拉曼光谱（FSRS），为各种光敏系统的结构-能量-功能关系提供了亮光。本《观点》回顾了结合光学创新的最新工作，包括将宽带上转换多色阵列（BUMA）集成到可调FSRS设置中，并展示了其观察金属形态和光解的分辨能力，从而产生了高质量的薄膜和荧光钙离子成像的嵌合蛋白生物传感器的调节。我们讨论了在混合时频域中执行FSRS的优势，并提出了通过跟踪低频模式并系统地修饰具有特定官能团的化学结构来描述机制的策略。这些在化学键方面的独特见解已开始实现光学，材料，能源和生命科学领域中功能分子机器的合理设计和精确控制。