Nanometric probes based on surface-enhanced Raman scattering (SERS) are promising candidates for all-optical environmental, biological and technological sensing applications with intrinsic quantitative molecular specificity. However, the effectiveness of SERS probes depends on a delicate trade-off between particle size, stability and brightness that has so far hindered their wide application in SERS imaging methodologies. In this Article, we introduce holographic Raman microscopy, which allows single-shot three-dimensional single-particle localization. We validate our approach by simultaneously performing Fourier transform Raman spectroscopy of individual SERS nanoparticles and Raman holography, using shearing interferometry to extract both the phase and the amplitude of wide-field Raman images and ultimately localize and track single SERS nanoparticles inside living cells in three dimensions. Our results represent a step towards multiplexed single-shot three-dimensional concentration mapping in many different scenarios, including live cell and tissue interrogation and complex anti-counterfeiting applications.

基于表面增强拉曼散射（SERS）的纳米探针具有固有的定量分子特异性，有望用于全光学环境，生物和技术传感应用。但是，SERS探针的有效性取决于颗粒大小，稳定性和亮度之间的微妙折衷，这迄今为止阻碍了它们在SERS成像方法学中的广泛应用。在本文中，我们介绍了全息拉曼显微镜，它允许单次三维单颗粒定位。我们通过同时执行单个SERS纳米粒子的傅里叶变换拉曼光谱和拉曼全息图来验证我们的方法，使用剪切干涉术提取宽视野拉曼图像的相位和幅度，并最终在三个维度上定位和跟踪活细胞内部的单个SERS纳米颗粒。我们的结果代表了在许多不同情况下向多路复用单次三维浓度分布图迈出的一步，包括活细胞和组织询问以及复杂的防伪应用。