Visualization of Vibrational Modes in Real Space by Tip-Enhanced Non-Resonant Raman Spectroscopy

被引:58
作者
Duan, Sai [1 ]
Tian, Guangjun [1 ]
Luo, Yi [1 ,2 ,3 ]
机构
[1] Royal Inst Technol, Sch Biotechnol, Dept Theoret Chem & Biol, S-10691 Stockholm, Sweden
[2] Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Anhui, Peoples R China
[3] Univ Sci & Technol China, Synerget Innovat Ctr Quantum Informat & Quantum P, Hefei 230026, Anhui, Peoples R China
基金
瑞典研究理事会;
关键词
ab initio calculations; Raman spectroscopy; surface chemistry; vibrational spectroscopy; water adsorption; WATER DISSOCIATION; CHEMICAL-ANALYSIS; SINGLE-MOLECULE; FIELD; RESOLUTION;
D O I
10.1002/anie.201508218
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
We present a general theory to model the spatially resolved non-resonant Raman images of molecules. It is predicted that the vibrational motions of different Raman modes can be fully visualized in real space by tip-enhanced non-resonant Raman scattering. As an example, the non-resonant Raman images of water clusters were simulated by combining the new theory and first-principles calculations. Each individual normal mode gives rise its own distinct Raman image, which resembles the expected vibrational motions of the atoms very well. The characteristics of intermolecular vibrations in supermolecules could also be identified. The effects of the spatial distribution of the plasmon as well as nonlinear scattering processes were also addressed. Our study not only suggests a feasible approach to spatially visualize vibrational modes, but also provides new insights in the field of nonlinear plasmonic spectroscopy.
引用
收藏
页码:1041 / 1045
页数:5
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