Surface-Enhanced Femtosecond Stimulated Raman Spectroscopy
Surface-Enhanced Femtosecond Stimulated Raman Spectroscopy
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DOI：
10.1021/jz200498z
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发表时间：
2011-05-19
影响因子：
5.7
通讯作者：
Van Duyne, Richard P.
中科院分区：
文献类型：
--
作者：
Frontiera, Renee R.;Henry, Anne-Isabelle;Van Duyne, Richard P.
表面增强拉曼光谱（SERS）和飞秒受激拉曼光谱（FSRS）彻底改变了拉曼光谱领域。 SERS 提供单分子的光谱检测，FSRS 能够在分子运动的超快时间尺度上采集拉曼光谱。在这里，我们首次成功结合了这两种技术，展示了使用嵌入报告分子的金纳米天线的表面增强飞秒受激拉曼光谱（SE-FSRS）。使用皮秒拉曼和飞秒探测脉冲，时间平均和整体平均增强因子估计在 10(4)-10(6) 范围内。我们报告了 SE-FSRS 信号的线形状、功率依赖性和幅度，并讨论了在分钟时间尺度上对样品降解的贡献。通过这些首次成功的原理验证实验，现在可以合理地尝试时间分辨 SE-FSRS 技术，以研究等离子体材料的动力学以及通过探测更同质的分子子集来检查环境异质性的贡献。
Surface-enhanced Raman spectroscopy (SERS) and femtosecond stimulated Raman spectroscopy (FSRS) have revolutionized the Raman spectroscopy field. SERS provides spectroscopic detection of single molecules, and FSRS enables the acquisition of Raman spectra on the ultrafast time scale of molecular motion. Here, we present the first successful combination of these two techniques, demonstrating surface-enhanced femtosecond stimulated Raman spectroscopy (SE-FSRS) using gold nanoantennas with embedded reporter molecules. Using a picosecond Raman and femtosecond probe pulse, the time- and ensemble-averaged enhancement factor is estimated to be in the range of 10(4)-10(6). We report the line shapes, power dependence, and magnitude of the SE-FSRS signal and discuss contributions to sample degradation on the minute time scale. With these first successful proof-of-principle experiments, time-resolved SE-FSRS techniques can now be rationally attempted with the goals of investigating the dynamics of plasmonic materials as well as examining the contributions of environmental heterogeneities by probing more homogeneous molecular subsets.