Stimulated Raman Photothermal Microscopy towards Ultrasensitive Chemical Imaging

Stimulated Raman scattering (SRS) microscopy has shown enormous potential in revealing<br> molecular structures, dynamics and couplings in complex systems. However, the sensitivity of SRS is<br> fundamentally limited to milli-molar level due to the shot noise and the small modulation depth. To<br> overcome this barrier, we revisit SRS from the perspective of energy deposition. The SRS process pumps<br> molecules to their vibrationally excited states. The thereafter relaxation heats up the surrounding and<br> induces refractive index changes. By probing the refractive index changes with a laser beam, we introduce<br> stimulated Raman photothermal (SRP) microscopy, where a &gt;500-fold boost of modulation depth is<br> achieved. Versatile applications of SRP microscopy on viral particles, cells, and tissues are demonstrated.<br> SRP microscopy opens a way to perform vibrational spectroscopic imaging with ultrahigh sensitivity. This dataset is the complete raw data used in the paper to support the findings.受激拉曼散射显微镜（Stimulated Raman scattering, SRS）已在揭示复杂系统中的分子结构、动力学特性与分子间耦合机制方面展现出巨大应用潜力。然而受激拉曼散射显微镜的灵敏度本质上受限于毫摩尔级别，这源于散粒噪声与较小的调制深度。为突破这一局限，我们从能量沉积的视角重新审视受激拉曼散射过程：受激拉曼散射过程可将分子泵浦至振动激发态，后续的弛豫过程会加热周围介质并引发折射率变化。通过利用激光束探测此类折射率变化，我们提出了受激拉曼光热显微镜（Stimulated Raman photothermal, SRP），其调制深度实现了500倍以上的提升。本研究验证了受激拉曼光热显微镜在病毒颗粒、细胞与组织样本中的多样化应用场景。受激拉曼光热显微镜为实现超高灵敏度的振动光谱成像提供了全新途径。本数据集即为支撑该论文研究结论的完整原始实验数据。