Cavendish Laboratory, Department of Chemical Engineering and Biotechnology, University of Cambridge, J. J. Thomson Avenue, Cambridge, CB3 0HE, United Kingdom.
Nano Lett. 2011 Dec 14;11(12):5339-43. doi: 10.1021/nl202875w. Epub 2011 Nov 18.
Coherent anti-Stokes Raman spectroscopy (CARS) is a well-known tool in multiphoton imaging and nonlinear spectroscopy. In this work we combine CARS with plasmonic surface enhancement on reproducible nanostructured surfaces. We demonstrate strong correlation between plasmon resonances and surface-enhanced CARS (SECARS) intensities on our nanostructured surfaces and show that an enhancement of ∼10(5) can be obtained over standard CARS. Furthermore, we find SECARS to be >10(3) times more sensitive than surface-enhanced Raman Spectroscopy (SERS). We also demonstrate SECARS imaging of molecular monolayers. Our work paves the way for reliable single molecule Raman spectroscopy and fast molecular imaging on plasmonic surfaces.
相干反斯托克斯拉曼光谱(CARS)是多光子成像和非线性光谱学中一种常用的工具。在这项工作中,我们将 CARS 与可重复的纳米结构表面上的等离子体表面增强相结合。我们在纳米结构表面上证明了等离子体共振与表面增强的 CARS(SECARS)强度之间的强相关性,并表明可以在标准 CARS 上获得约 10(5)倍的增强。此外,我们发现 SECARS 的灵敏度比表面增强拉曼光谱(SERS)高 10(3)倍以上。我们还演示了分子单层的 SECARS 成像。我们的工作为在等离子体表面上进行可靠的单分子拉曼光谱和快速分子成像铺平了道路。