等离子体衰变动力学与表面增强拉曼光谱背景之间的联系:非热和热载流子的非弹性散射

Shengxian Wu, Oscar Hsu-Cheng Cheng, B. Zhao, Nicki Hogan, An-Tse Lee, D. Son, M. Sheldon
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引用次数: 6

摘要

最近的研究已经证实,等离子体金属纳米结构的反斯托克斯拉曼信号可以用来确定金属内部载流子的两个不同温度——光激发“热载流子”的温度和与金属晶格热化的载流子的温度。然而,Stokes光谱区域的相关信号历来阻碍了表面增强拉曼光谱(SERS),因为吸附分子的振动峰总是伴随着金属衬底的宽背景。金属信号的基本来源,以及它对频谱的贡献,一直不清楚。在这里,我们概述了一个统一的理论模型,描述了温度依赖的行为和广谱分布。我们认为,大部分拉曼信号是直接与非热载流子的非弹性散射,这些载流子是通过表面等离子体激元的阻尼激发的。此外,显著的光谱成分(~ 1%)是由于热分布中热载流子的亚群。我们进行了温度和功率相关的拉曼实验,展示了一个简单的拟合程序如何揭示等离子体脱相时间,以及热载流子和金属晶格的温度,以便将这些参数与吸附在金属表面的化学物质的定量拉曼分析联系起来。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
The connection between plasmon decay dynamics and the surface enhanced Raman spectroscopy background: Inelastic scattering from non-thermal and hot carriers
Recent studies have established that the anti-Stokes Raman signal from plasmonic metal nanostructures can be used to determine the two separate temperatures that characterize carriers inside the metal -- the temperature of photoexcited "hot carriers" and carriers that are thermalized with the metal lattice. However, the related signal in the Stokes spectral region has historically impeded surface enhanced Raman spectroscopy (SERS), as the vibrational peaks of adsorbed molecules are always accompanied by the broad background of the metal substrate. The fundamental source of the metal signal, and hence its contribution to the spectrum, has been unclear. Here, we outline a unified theoretical model that describes both the temperature-dependent behavior and the broad spectral distribution. We suggest that the majority of the Raman signal is from inelastic scattering directly with non-thermal carriers that have been excited via damping of the surface plasmon. In addition, a significant spectral component (~ 1%) is due to a sub-population of hot carriers in an elevated thermal distribution. We have performed temperature and power-dependent Raman experiments to show how a simple fitting procedure reveals the plasmon dephasing time, as well as the temperatures of the hot carriers and the metal lattice, in order to correlate these parameters with quantitative Raman analysis of chemical species adsorbed on metal surface.
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