单光束相干喇曼光谱和显微镜的陷波整形
Single-Beam Coherent Raman Spectroscopy and Microscopy via Spectral Notch Shaping
摘要：
拉曼光谱是研究分子振动模式和结构的关键技术之一。在相干反斯托克斯拉曼散射（CARS）光谱中，分子振动光谱通过泵浦、斯托克斯和探测光子的三阶非线性相互作用来解析，通常使用具有多个光束和激光源的复杂实验装置。虽然CARS已经成为一种广泛应用的无标记化学成像和污染物检测技术，但其多源，多光束实验实施具有挑战性。在这项工作中，我们提出了一个简单的，易于实施的计划进行单光束CARS光谱和显微镜使用一个单一的飞秒脉冲，由一个可调窄带陷波滤波器成形。作为多源的替代，单个宽带脉冲同时提供泵浦、斯托克斯和探测光子，激发宽带振动能级。利用谐振光子晶体板状滤波器形成的可调谐光谱陷波作为窄带延时探针，获得了高光谱分辨率。使用该方案，整个振动频谱可以在单次多路复用测量中解析，从而避免了对多源配置或复杂脉冲整形装置的需要。我们展示了在300 cm ^{-1}-1000 cm ^{-1}光谱范围内的各种样品的高分辨率单光束显微光谱和振动成像。
英文摘要：
Raman spectroscopy is one of the key techniques in the study of vibrational modes and molecular structures. In Coherent Anti-Stokes Raman Scattering (CARS) spectroscopy, a molecular vibrational spectrum is resolved via the third-order nonlinear interaction of pump, Stokes and probe photons, typically using a complex experimental setup with multiple beams and laser sources. Although CARS has become a widespread technique for label-free chemical imaging and detection of contaminants, its multi-source, multi-beam experimental implementation is challenging. In this work we present a simple and easily implementable scheme for performing single-beam CARS spectroscopy and microscopy using a single femtosecond pulse, shaped by a tunable narrowband notch filter. As a substitute for multiple sources, the single broadband pulse simultaneously provides the pump, Stokes and probe photons, exciting a broad band of vibrational levels. High spectroscopic resolution is obtained by utilizing a tunable spectral notch, shaped with a resonant photonic crystal slab filter, as a narrowband, time-delayed probe. Using this scheme the entire vibrational spectrum can be resolved in a single-shot multiplexed measurement, circumventing the need for a multi-source configuration or a complex pulse-shaping apparatus. We demonstrate high-resolution single-beam micro-spectroscopy and vibrational imaging of various samples in the 300cm^{-1}-1000cm^{-1} spectral range.
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