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In non-relativistic quantum electrodynamics, an electromagnetic (EM)interaction between a photon and a molecular exciton can be expressed by a Apterm and A^2 term, where A and p are the operators of the vector potential ofthe EM field and the momentum of the exciton, respectively. We developed amethod for investigating the contribution of the Ap and A^2 terms to EMenhancement, which occurs in coupled systems composed of a plasmon polaritonand a molecular exciton. The spectral shapes of the Ap and A^2 terms terms, andthe EM enhancement were experimentally obtained from absorption, Rayleighscattering, and ultrafast surface enhanced fluorescence (ultrafast SEF) of thesystems, respectively. The relationships between them reveal that theabsorption spectra correctly reproduce EM enhancement, indicating thatultrafast SEF can be described as a two-step process using the Ap term.Furthermore, we demonstrate that the origin of spectral deviation betweenRayleigh scattering and EM enhancement is subradiant plasmon resonance, whichspectra are visualized in the absorption not in Rayleigh scattering, withnumerical calculation based on electromagnetism.

journal of chemical physics online/the journal of chemical physics/journal of chemical physics

Electromagnetic enhancement generated by Ap term of cavity quantum  electrodynamics demonstrated by single coupled systems between plasmon and  molecular exciton