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Quantum theory of surface-enhanced resonant Raman scattering (SERRS) of molecules in strongly coupled plasmon–exciton systems by Tomáš Neuman; Javier Aizpurua; Ruben Esteban is a Engineering article available to read on EtoBox.

What is Quantum theory of surface-enhanced resonant Raman scattering (SERRS) of molecules in strongly coupled plasmon–exciton systems about?

Localised surface plasmons can couple strongly with the electronic transitions of a molecule, inducing new hybridised states of light and matter, the plasmon-exciton polaritons. Furthermore, molecules support vibrational degrees of freedom that interact with the electronic levels, giving rise to inelastic resonant Raman scattering under coherent laser illumination. Here we show the influence of strong plasmon-exciton coupling on resonant Raman processes that populate the vibrational states of the molecule and that lead to the characteristic surface-enhanced Raman scattering spectra. We develop analytical expressions that give insight into these processes for the case of moderate illumination intensity, weak electron-vibration coupling and no dephasing. These expressions help us to elucidate the twofold role of plasmon-exciton polaritons to pump the system efficiently and to enhance the Raman emission. Our results show a close analogy with the optomechanical process described for off-resonant Raman scattering but with a difference in the resonant reservoir. We also use full numerical calculations to study the effects reaching beyond these approximations and discuss the interplay bet

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Author

Tomáš Neuman; Javier Aizpurua; Ruben Esteban

Publisher

Walter de Gruyter GmbH

Published

2020

Language

EN

Field

Engineering (Physical Sciences)