Molecule-Dependent Plasmonic Enhancement of Fluorescence and Raman Scattering near Realistic Nanostructures外文.pdf

ARTICLE Molecule-Dependent Plasmonic Enhancement of Fluorescence and Raman Scattering near Realistic Nanostructures Andreas M. Kern,?,?,* Alfred J. Meixner,? and Olivier J. F. Martin?,* ?Nanophotonics and Metrology Laboratory, Swiss Federal Institute of Technology Lausanne (EPFL), 1015 Lausanne, Switzerland and ?Institute of Physical and Theoretical Chemistry, Eberhard Karls University, 72076 Tübingen, Germany In the past decade, the localized enhancement of ?uorescence processes and Raman scattering has materialized as a model application of plasmonic nanostructures.1à16 Tuned to the right wavelength, such a nanostructure acts as an antenna, leading to an enhancement of the incident, exciting radiation as well as amplifying the light reemitted by the molecule. The obtained increase in signal can be used to make visible weak radiative processes, for example, in biological systems17à20 or organic semiconductors.21 To quantify the e?ciency of this approach, an enhancement factor can be de?ned which compares the measurable signal, in most settings the optical power radiated to the far-?eld, for the case of a molecule near an enhancing structure with that of the same molecule in free space. The total enhancement factor is the result of a balance between various processes pertaining to both the excitation and reemission of light and depends on many properties of the molecule as well as the plasmonic structure. Various models have been presented to predict the enhancement factors near rough metal surfaces22 and metal nanoparticles.23à26 These models give interesting insight into the factors which a?ect enhancement, but make assumptions regarding either the molecules transition rates25,26 or intrinsic quantum yield.25 In addition, the e?ect of the plasmonic nanostructure is described using either empirical values22,23 or a simpli?ed analytical model.17à19,25à27 While analytical models may produce elegant descriptions of complex phenomena and can aid in the comprehension of