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Visualization of Vibrational Modes in Real Space by Tip‐Enhanced Non‐Resonant Raman Spectroscopy
Author(s) -
Duan Sai,
Tian Guangjun,
Luo Yi
Publication year - 2016
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.201508218
Subject(s) - raman spectroscopy , raman scattering , coherent anti stokes raman spectroscopy , plasmon , molecular vibration , normal mode , intermolecular force , molecular physics , x ray raman scattering , resonance (particle physics) , nonlinear system , infrared , spectroscopy , vibration , molecule , chemistry , optics , atomic physics , physics , quantum mechanics
Abstract 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.