3-color coherent anti-Stokes Raman scattering with optical non-resonant background removal

3-color coherent anti-Stokes Raman scattering with optical non-resonant background removal
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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:
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发表时间:
2019
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通讯作者:
D. Richards
D. Richards
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作者:
Priyank Shah;Thomas Kavanagh;D. Richards

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宽带相干反斯托克斯拉曼散射(B-CARS),通过脉冲内三色过程激发,其中泵浦和斯托克斯光子都来自宽带光束,使整个指纹光谱区域的衍射限制高光谱拉曼成像的速度和灵敏度远远优于传统的自发拉曼共聚焦微光谱学。我们将光谱干涉偏振相干反斯托克斯拉曼散射(SIP-CARS)理论扩展到包括三色激发过程。这使得B-CARS测量偏振拉曼等效光谱没有非谐振背景,不需要采集后的计算处理。我们演示了同时测量三色和两色SIP-CARS,分别在低和高拉曼位移下,与理论很好地一致。这些概念验证结果为利用超快激光器产生光子高效SIP-CARS信号、实现全光学、快速、定量拉曼高光谱成像铺平了道路。
Broadband coherent anti-Stokes Raman scattering (B-CARS), excited through intra-pulse 3-color processes in which both the pump and Stokes photons are derived from a broadband beam, enables 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 micro-spectroscopy. We extend the theory of spectral interferometric polarization coherent anti-Stokes Raman scattering (SIP-CARS) to include 3-color excitation processes. This allows for the B-CARS measurement of polarized Raman-equivalent spectra free of the non-resonant background, without the requirement for post-acquisition computational processing. We demonstrate the simultaneous measurement of both 3-color and 2color 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.