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Plasmonics: Design, Materials, Fabrication, Characterization, and Applications

Cavity-modified fluorescence in the weak and strong coupling regimes

Momil Baig, Wonmi Ahn

Published Aug 1, 2025• 0 citations
Publisher

Abstract

In this study, we demonstrate that the fluorescence of fluorescein dye molecules can be significantly modified in both the weak and strong coupling regimes by placing the molecules inside a perturbative or non-perturbative Fabry-Pérot cavity. By controlling the cavity thickness and dye concentration, we selectively altered the frequency and number of cavity transmission peaks, thereby establishing conditions for weak or strong coupling for fluorescein molecules. Using steady-state fluorescence spectroscopy, we confirmed that both the excitation and emission spectra were substantially tuned in these coupling regimes, enabling tunable and multicolor fluorescence from a single type of dye molecule, fluorescein.

DOI
10.1117/12.3064042

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In this study, we demonstrate that the fluorescence of fluorescein dye molecules can be significantly modified in both the weak and strong coupling regimes by placing the molecules inside a perturbative or non-perturbative Fabry-Pérot cavity. By controlling the cavity thickness and dye concentration, we selectively altered the frequency and number of cavity transmission peaks, thereby establishing conditions for weak or strong coupling for fluorescein molecules. Using steady-state fluorescence spectroscopy, we confirmed that both the excitation and emission spectra were substantially tuned in these coupling regimes, enabling tunable and multicolor fluorescence from a single type of dye molecule, fluorescein.
Abstract Light–matter interaction leads to excitation of molecules, which, in turn, can exchange energy with a localized electromagnetic field. This can be used for engineering of the electronic and vibrational energy levels of the molecules. This study considers the conditions for the emergence of the strong light–matter coupling regime for organic dye molecules in a tunable Fabry–Perot microcavity formed by a convex mirror and a flat reflecting surface. The sample studied was made of hexagonal boron nitride (hBN), polyvinylpyrrolidone polymer (PVP, 55 kDa), and rhodamine 6G fluorophore (R6G). Strong light–matter coupling was obtained in a sample with a low concentration of PVP. Adjustment of the optical path length in the microcavity by varying the thickness of the hBN–R6G–PVP film made it possible to obtain a high density of modes in the cavity (several tens of (λ/n)3) and, hence, to study the weak and strong light–matter coupling regimes. The results offer the possibility of studying the basic mechanisms of resonant light–matter interaction at room temperature, as well as developing new practical applications of the strong coupling effect.
The interaction of light and matter in a microcavity depends crucially on the position of the emitter in the spatial field distribution of the resonator mode. In an ideal experiment one would like to place an emitter at will within the mode of the cavity to change the interaction strength in a controllable fashion. Although several efforts have aimed at the realization of such a scheme, its application remains an experimental challenge. Fabry-Perot microresonators constitute a promising route for a controlled coupling of atoms in the gas phase as well as for solid state systems and molecules. Here we present the selective coupling of fluorescent nanoparticles and single molecules to a tunable, fiber-based, scannable microcavity.
Coupling of macroscopic ensembles of highly concentrated R6G molecules with aluminum and silver Fabry–Perot cavities of different sizes, in which one or two standing wave modes are in resonance with the absorption transition(s) of the dye molecules, have been studied. (i) It has been found that strong coupling of the cavity with one molecular eigenstate (S0→S1 transition) does not perturb the energies of the other molecular states. (ii) The S0→S2 absorption transition is too weak to strongly couple to the resonant cavity (“λ” standing wave mode). However, the resonant cavity causes a blue shift of the S0→S2 excitation band. (iii) The splitting of the dispersion curve is theoretically predicted and experimentally observed at strong coupling of the cavity resonance (“λ” standing wave mode) with the material resonances of Ag, including bound electron and “epsilon equal zero” transitions.
We investigate experimentally and theoretically the fluorescence emitted by molecular ensembles as well as spatially isolated, single molecules of an organic dye immobilized in a quasi-planar optical microresonator at room temperature. The optically excited dipole emitters couple simultaneously to on- and off-axis cavity resonances of the microresonator. The multi-spectral radiative contributions are strongly modified with respect to free (non-confined) space due to enhancement and inhibition of the molecular spontaneous emission (SpE) rate. By varying the mirror spacing of the microresonator on the nanometer-scale, the SpE rate of the cavity-confined molecules and, consequently, the spectral line width of the microresonator-controlled broadband fluorescence can be tuned by up to one order of magnitude. Stepwise reducing the optical confinement, we observe that the microresonator-controlled molecular fluorescence line shape converges towards the measured fluorescence line shape in free space. Our results are important for research on and application of broadband emitters in nano-optics and -photonics as well as microcavity-enhanced (single molecule) spectroscopy.