Three-color coherent anti-Stokes Raman scattering with optical nonresonant background removal
Three-color coherent anti-Stokes Raman scattering with optical nonresonant background removal
复制标题
具有光学非共振背景去除功能的三色相干反斯托克斯拉曼散射
DOI：
10.1002/jrs.5576
复制
发表时间：
2019
影响因子：
2.5
通讯作者：
Littleton B
中科院分区：
文献类型：
--
作者：
Littleton B
宽带相干反斯托克斯拉曼散射（B）通过脉冲内三色过程激发，其中泵浦光子和斯托克斯光子都来自宽带光束，能够在整个指纹光谱区域进行衍射限制的高光谱拉曼成像，其速度和灵敏度远远上级传统的自发拉曼共焦显微光谱。我们扩展了光谱干涉偏振相干反斯托克斯拉曼散射（SIP‐汽车）的理论，包括三色激发过程。这使得B-汽车测量偏振拉曼-等效光谱的非共振背景，而无需采集后的计算处理。我们证明了三色和双色SIP‐汽车的同时测量，分别在低和高拉曼位移，与理论吻合得很好。这些概念验证结果为使用超快激光器产生光子高效的SIP‐汽车信号铺平了道路，用于全光学，快速，定量拉曼高光谱成像。
Broadband coherent anti‐Stokes Raman scattering (B‐CARS), excited through intrapulse three‐color processes in which both the pump and Stokes photons are derived from a broadband beam, enable diffraction‐limited hyperspectral Raman imaging over the entire fingerprint spectral region with a speed and sensitivity far superior to that possible with conventional spontaneous Raman confocal microspectroscopy. We extend the theory of spectral interferometric polarization coherent anti‐Stokes Raman scattering (SIP‐CARS) to include three‐color excitation processes. This allows for the B‐CARS measurement of polarized Raman‐equivalent spectra free of the nonresonant background, without the requirement for post‐acquisition computational processing. We demonstrate the simultaneous measurement of both three‐color and two‐color SIP‐CARS, at low and high Raman shifts, respectively, in good agreement with theory. These proof of concept results pave the way for photon‐efficient SIP‐CARS signal generation with ultrafast lasers, for all‐optical, fast, quantitative Raman hyperspectral imaging.