{ "id": "1406.3695", "version": "v3", "published": "2014-06-14T07:27:16.000Z", "updated": "2014-10-09T08:23:47.000Z", "title": "Raman Images of a Single Molecule in a Highly Confined Plasmonic Field", "authors": [ "Sai Duan", "Guangjun Tian", "Yongfei Ji", "Jiushu Shao", "Yi Luo" ], "comment": "5 pages, 4 figures, Revised version", "categories": [ "cond-mat.mes-hall", "physics.optics" ], "abstract": "Under the local plasmonic excitation, the Raman images of a single molecule can now reach sub-nm resolution. We report here a description for the interaction between a molecule and a highly confined plasmonic field. It is shown that when the spatial distribution of the plasmonic field is comparable with the size of the molecule, the optical transition matrix of the molecule becomes to be dependent on the position and distribution of the plasmonic field, resulting in spatially resolved Raman image of a molecule. It is found that the resonant Raman image reflects the electronic transition density of the molecule. In combination with the first principles calculations, the simulated Raman image of a porphyrin derivative adsorbed on the silver surface nicely reproduces its experimental counterpart. The present theory provides the basic framework for describing linear and nonlinear responses of molecules under the highly confined plasmonic field.", "revisions": [ { "version": "v2", "updated": "2014-06-18T08:41:38.000Z", "abstract": "Under the local plasmonic excitation, the Raman images of a single molecule can now reach sub-nm resolution. We report here a general theory to describe the interaction between a molecule and a highly confined plasmonic field. It is shown that when the spatial distribution of the plasmonic field is comparable with the size of the molecule, the plasmonic field needs to be treated quantum mechanically. The resonant Raman image of a molecule is found to be strongly associated with the density of the electronic transition. In combination with the first principles calculations, the simulated Raman image of a porphyrin derivative adsorbed on the silver surface nicely reproduces its experimental counterpart. It reveals that the quantum nature of the highly confined plasmonic field offers a new way to modify the wavefunction of the molecule. The present theory provides the basic framework for describing linear and nonlinear responses of molecules under the non-uniform quantized field.", "comment": "5 pages, 4 figures", "journal": null, "doi": null }, { "version": "v3", "updated": "2014-10-09T08:23:47.000Z" } ], "analyses": { "keywords": [ "single molecule", "resonant raman image", "first principles calculations", "silver surface nicely reproduces", "highly confined plasmonic field offers" ], "note": { "typesetting": "TeX", "pages": 5, "language": "en", "license": "arXiv", "status": "editable", "adsabs": "2014arXiv1406.3695D" } } }