Enhancement of Raman scattering for an atom or molecule near a metal nanocylinder: Quantum theory of spontaneous emission and coupling to surface plasmon modes

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Abstract
An analytic expression for the electromagnetic enhancement of the spontaneous emission rate and Raman scattering cross-section for an excited atom or molecule in close proximity to a metal nanocylinder has been derived by quantum theory. Coupling of the atomic or molecular optical radiation into the TM0 surface plasmon mode of the nanocylinder results in reradiation by the cylinder, a process that is most efficient when the incident radiation is linearly polarized, with the electric field oriented parallel to the axis of the nanocylinder. For a silver cylinder having a radius and length of 5 and 20nm, respectively, the enhancement in the spontaneous emission rate is >107 for ℏω0≃2.4eV (λ=514nm), which corresponds to an increase of ≈1014 in the Raman scattering cross section. This result, as well as the prediction that the atomic dipole generates broadband, femtosecond pulses, are in qualitative agreement with previously reported experiments involving metal nanoparticle aggregates. The theoretical results described here are expected to be of value in guiding future nonlinear optical experiments in which carbon nanotubes or metal nanowires with controllable physical and electrical characteristics are patterned onto a substrate and coupled with emitting atoms or molecules.