Probing Vibrational Strong Coupling of Molecules with Wavelength-Modulated Raman Spectroscopy,Advanced Optical Materials

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Probing Vibrational Strong Coupling of Molecules with Wavelength-Modulated Raman Spectroscopy
Advanced Optical Materials ( IF 8.0 ) Pub Date : 2021-11-27 , DOI: 10.1002/adom.202102065
Kishan S. Menghrajani ₁ , Mingzhou Chen ₂ , Kishan Dholakia ₂ , William L. Barnes ₁

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Raman spectroscopy is a powerful technique that enables fingerprinting of materials, molecules, and chemical environments by probing vibrational resonances. In many applications, the desired Raman signals are masked by fluorescence, either from the molecular system being studied, or from adjacent metallic nanostructures. Here, it is shown that wavelength-modulated Raman spectroscopy provides a powerful way to significantly reduce the strength of the fluorescence background, thereby allowing the desired Raman signals to be clearly recorded. This approach is made use of to explore Raman scattering in the context of vibrational strong coupling, an area that has thus far been problematic to visualise. Specifically, strong coupling between the vibrational modes in a polymer and two types of confined light field, the fundamental mode of a metal-clad microcavity, and the surface-plasmon modes of an adjacent thin metal film are looked at. While clear advantages in using the wavelength-modulated Raman approach are found, these results on strong coupling are inconclusive, and highlight the need for more work in this exciting topic area.

中文翻译：

用波长调制拉曼光谱探测分子的振动强耦合

拉曼光谱是一种强大的技术，可以通过探测振动共振来对材料、分子和化学环境进行指纹识别。在许多应用中，所需的拉曼信号被荧光所掩盖，无论是来自正在研究的分子系统，还是来自相邻的金属纳米结构。在这里，它表明波长调制拉曼光谱提供了一种有效的方法来显着降低荧光背景的强度，从而可以清楚地记录所需的拉曼信号。这种方法用于在振动强耦合的背景下探索拉曼散射，这是迄今为止难以可视化的一个领域。具体来说，聚合物中的振动模式与两种类型的受限光场之间的强耦合，研究了金属包层微腔的基本模式，以及相邻金属薄膜的表面等离子体模式。虽然发现了使用波长调制拉曼方法的明显优势，但这些关于强耦合的结果尚无定论，并强调需要在这个令人兴奋的主题领域开展更多工作。

更新日期：2021-11-27

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