Combining Optical Strong Mode Coupling with Polaritonic Coupling in a λ/2 Fabry–Pérot Microresonator

Abstract

Strong coupling has attracted much research interest motivated by the possibility to tune the energy levels of molecules enabling to control and modify chemical reactions. Strong coupling leads to the formation of new hybrid modes and is caused by coherent energy exchange between the individual constituents. Such a coherent energy exchange occurs when the coupling rate exceeds the damping rate of the individual components and has been observed for highly diverse systems. Here, we present a strongly coupled hybrid system consisting of a thin TDBC J-aggregate film inside an optical subwavelength microresonator coupled to a second microresonator. This hybrid structure combines strong coupling of purely optical modes with strong light–matter interaction. The coupling strength and damping sensitively depend on the position and concentration of the coupled molecules in the microresonator structure. Such a coupled system can be modeled by coupled damped oscillators, which allows to determine the coupling and damping constants. We show that the individual components making up the coupled hybrid system cannot be treated individually, but the coupled system needs to be considered as a whole. As a consequence, altering one parameter does influence the whole coupled system, and the individual components need to be carefully adapted to each other to achieve efficient coupling. These results can have important consequences for the field of optoelectronics or polaritonic chemistry.

Controlling Three-Color Förster Resonance Energy Transfer in an Optical Fabry–Pérot Microcavity at Low Mode Order

“…Single nanospheres were deposited with an average separation of several micrometers on top of a 100 nm thick SiO 2 spacer layer on the tunable mirror. 75 The optical path length of the microcavity can be tuned by precisely approaching the tunable mirror toward the fixed mirror by piezoelectric actuators.…”

“…To investigate the influence of the optical microcavity on the radiative properties of the dyes, fluorescent nanospheres were embedded between the two mirrors of the tunable microcavity, as schematically presented in Figure b. Single nanospheres were deposited with an average separation of several micrometers on top of a 100 nm thick SiO 2 spacer layer on the tunable mirror . The optical path length of the microcavity can be tuned by precisely approaching the tunable mirror toward the fixed mirror by piezoelectric actuators.…”

“…The tunable flat mirror is created by evaporating a 50 nm thick silver layer on a clean glass cover slide, followed by a 10 nm gold and a dielectric SiO 2 layer of 100 nm to position the nanospheres. In this way, we avoid fluorescence quenching by the silver mirror , and make sure that the fluorophores are located in the first spatial intensity maximum of the cavity modes and experience a high field strength. The fixed mirror is a lens with a curvature radius of 18.6 mm, coated with an 80 nm silver layer, a 10 nm thick gold layer, and 20 nm SiO 2 as a protection layer.…”

Hyperspectral Imaging of Exciton Polaritons in Optical Microcavities

“…20 To observe the strong coupling regime in microcavities, it is crucial to precisely tune the cavity photon energy to match the resonance energy of the excitons placed inside the optical microcavity. For example, in recent studies, 21,22 in the strong coupling regime, a piezo actuator has been successfully utilized to modify the detuning between the cavity resonance mode and the excitons by adjusting the distance between the cavity mirrors. This manipulation allows observation of a strong coupling regime in the interaction between the cavity light and excitons and facilitates the study of the interaction between different photon energies and the excitonic source within the optical cavity.…”

Raman investigation of local photo‐bleaching in TDBC dye layer for photonics applications

“…[3] Advantage can also be taken from photo-bleaching like for mobility measurement in biology [4] or for tetrachloro diethyl benzimidazolo carbocyanine (TDBC) dye. For TDBC Jaggregated layers, photo-bleaching is widely used for strong coupling studies [5][6][7][8][9] and more recently for wavelength selective grating fabrication. [10] Indeed, TDBC dye layers have very interesting optical properties because they have a high oscillator strength at around 590-nm wavelength, [11][12][13] which can be suppressed under illumination.…”