High Fidelity Nano-Hole Enhanced Raman Spectroscopy.
High Fidelity Nano-Hole Enhanced Raman Spectroscopy.
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DOI：
10.1021/jp900764a
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发表时间：
2009-07-02
期刊：
影响因子：
--
通讯作者：
Chen L
中科院分区：
文献类型：
--
作者：
Bahns JT;Guo Q;Montgomery JM;Gray SK;Jaeger HM;Chen L
表面增强拉曼光谱（Sers）是一种灵敏的技术，甚至可以检测单个分子。然而，在许多Sers应用中，强局部场的强烈不均匀分布使得很难定量评估信号的保真度或再现性，这限制了Sers的应用。在这里，我们报告的发展异常高保真孔增强拉曼光谱（HERS）从有序的，二维六边形纳米孔阵列。我们将保真度f作为测量之间拉曼峰的百分比偏差的量度。总体而言，对于使用水性R6 G分子的HERS，12个金阵列样品的面积平均结晶度范围为f ~ 2% - 15%。此外，增强的拉曼光谱的强度调制的偏振角的函数首次被测量。这些测量中最好的测量集中在样品上的静态激光光斑上，可以与比面积平均结果更高的结晶度相一致。银中的纳米孔阵列提供了支持偏振测量和更完整的苯丙氨酸分子的增强拉曼指纹。我们还进行了时域有限差分计算，以协助解释的实验，确定可能产生的孔-孔相互作用的偏振依赖性。我们的结果代表了使定量和可重复的增强拉曼测量成为可能的一步，也为高度均匀热点的大规模来源开辟了新的途径。
Surface Enhanced Raman Spectroscopy (SERS) is a sensitive technique that can even detect single molecules. However, in many SERS applications, the strongly inhomogeneous distribution of intense local fields makes it very difficult for a quantitive assessment of the fidelity, or reproducibility of the signal, which limits the application of SERS. Herein we report the development of exceptionally high fidelity Hole-Enhanced Raman Spectroscopy (HERS) from ordered, two-dimensional hexagonal nanohole arrays. We take the fidelity f to be a measure of the percent deviation of the Raman peaks from measurement to measurement. Overall, area averaged fidelities for 12 gold array samples ranged from f ~ 2% – 15% for HERS using aqueous R6G molecules. Furthermore, intensity modulations of the enhanced Raman spectra were measured for the first time as a function of polarization angle. The best of these measurements, which focus on static laser spots on the sample, could be consistent with even higher fidelities than the area-averaged results. Nanohole arrays in silver provided supporting polarization measurements and a more complete enhanced Raman fingerprint for phenylalanine molecules. We also carried out finite-difference time-domain calculations to assist in the interpretation of the experiments, identifying the polarization dependence as possibly arising from hole-hole interactions. Our results represent a step towards making quantitative and reproducible enhanced Raman measurements possible and also open new avenues for a large scale source of highly uniform hot spots.
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