Modification of transition pathways in polarized resonance Raman spectroscopy for carbon nanotubes by highly confined near-field light

Yuto Fujita, Norihiko Hayazawa, Maria Vanessa Balois-Oguchi, Takuo Tanaka, Tomoko K. Shimizu
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Abstract

We observed a modification of transition pathways in polarized resonance Raman spectroscopy during tip-enhanced Raman spectroscopy (TERS) analysis of metallic carbon nanotubes (CNTs). At a spatial resolution reaching up to the sub-nanometer regime, the signal intensity of the typical D-band is observed to be even higher than the intensity of the G-band all over the probed CNTs in TERS imaging. The measured D-band is attributed to the non-vertical transitions of electrons in k-space that are facilitated by highly confined near-field light at the tip–sample junction of our scanning tunneling microscope based TERS system. The D-band signal was observed even when the CNTs were excited by light polarized perpendicular to the tube axis that corresponds to electronic excitations between different cutting line numbers of a CNT. By combining the electron pathways brought about by both the near-field light and its polarization, we found a unique optical transition of electrons of CNTs in near-field Raman spectroscopy.
高约束近场光改变碳纳米管偏振共振拉曼光谱的转变路径
在对金属碳纳米管(CNTs)进行针尖增强拉曼光谱(TERS)分析时,我们观察到偏振共振拉曼光谱的转变路径发生了变化。在空间分辨率达到亚纳米级的情况下,在 TERS 成像中观察到典型的 D 波段信号强度甚至高于整个探测 CNT 的 G 波段信号强度。测量到的 D 波段归因于电子在 k 空间的非垂直跃迁,这种跃迁在我们基于扫描隧道显微镜的 TERS 系统的尖端-样品交界处的高度约束近场光中得到了促进。即使 CNT 被垂直于管轴的偏振光激发,也能观察到 D 波段信号,这与 CNT 不同切割线数之间的电子激发相对应。通过结合近场光及其偏振带来的电子路径,我们发现了近场拉曼光谱中独特的 CNT 电子光学转变。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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