Vacuum Rabi Splitting and Strong-Coupling Dynamics for Surface-Plasmon Polaritons and Rhodamine 6G Molecules

Abstract

We report on strong coupling between surface-plasmon polaritons (SPP) and Rhodamine 6G (R6G) molecules, with double vacuum Rabi splitting energies up to 230 and 110 meV. In addition, we demonstrate the emission of all three energy branches of the strongly coupled SPP-exciton hybrid system, revealing features of system dynamics that are not visible in conventional reflectometry. Finally, in analogy to tunable-Q microcavities, we show that the Rabi splitting can be controlled by adjusting the interaction time between waveguided SPPs and R6G deposited on top of the waveguide. The interaction time can be controlled with sub-fs precision by adjusting the length of the R6G area with standard lithography methods.

Spatial modulation of light transmission through a single microcavity by coupling of photosynthetic complex excitations to surface plasmons

“…T he interaction between molecules and surface plasmons (SP) in defined geometries can lead to new light-matter hybrid states, where light propagation is strongly influenced by molecular photon absorption [1][2][3][4][5][6][7][8][9][10][11][12][13][14] . This phenomenon has been observed in organic semiconductor optical microcavities 3,[11][12][13] , sub-wavelength hole arrays 1,9,10 and molecules deposited on patterned surfaces 1 .…”

“…This phenomenon has been observed in organic semiconductor optical microcavities 3,[11][12][13] , sub-wavelength hole arrays 1,9,10 and molecules deposited on patterned surfaces 1 . The applications range from lasing 15 , LED's 12 , control of chemical reactions 11 and light harvesting 2,16,17 .…”

Exciton-plasmon coupling interactions: from principle to applications

“…The resonance exchange energy occurs between the upper and lower levels of the newly formed hybrid state (also called Rabi oscillation), which can be described as strong coupling. The strong coupling phenomenon can be proven by Rabi splitting in the stability spectrum [59] and the anticrossing phenomenon of the energy corresponding to the splitting peak at different coupling intensities [60]. When we talk about using SPs to promote absorption [61], SERS effects [62], fluorescence [63], and fluorescence quenching [64], the interaction that has no perturbation between wave functions can be called as weak coupling.…”

Efficient optical coupling into a single plasmonic nanostructure using a fiber-coupled microspherical cavity

“…LSP fields with the small mode volumes strongly enhance the interactions between light and matter [4][5][6][7][8]. Recently, vacuum Rabi splitting was observed in exciton-plasmon coupling systems at room temperature [9][10][11]. This effect demonstrates that a single photon harvested by the LSP antenna can couple into a single-exciton state with high efficiency, which will be applicable to highly efficient photonic devices.…”

“…We successfully demonstrate the 93% PL coupling into the LSP antenna with an effective area of a 58 nm circle, exceeding the diffraction limit. Localized surface plasmons (LSPs) of metal nanostructures have attracted considerable attention because of the unique enhancement of the exciton-photon coupling by strong localization of the optical field [1][2][3][4][5][6][7][8][9][10][11]. The LSP polaritons have the ability to confine the optical field into nanometer-scale areas, exceeding the diffraction limit, using the so-called optical antenna effect [1][2][3].…”