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Applied Physics Letters

Observation of ultrastrong-coupling regime in the Fabry–Pérot microcavities made of metal mirrors containing Lemke dye

Makoto Suzuki, Kouichi Nishiyama, Nobutaka Kani, Xinping Yu, Keiji Uzumi, Masahiro Funahashi, Fusao Shimokawa, Shunsuke Nakanishi, Noriaki Tsurumachi

Published May 13, 2019• 16 citations
Publisher

Abstract

We investigate the transmission properties of Fabry–Pérot microcavities made of metal mirrors containing the organic dye molecule, generally called Lemke. We synthesized Lemke dye and fabricated the microcavities by using simple vacuum evaporation and spin-coating methods. The vacuum Rabi splitting energy increases in proportion to the square root of the absorption coefficient of the cavity layers and exceeds 1 eV at maximum. The ratio of the vacuum Rabi splitting energy to the matter transition energy reaches 0.42, so we consider that the ultrastrong-coupling regime was attained. The dispersion relation is reasonably interpreted by using the full Hopfield Hamiltonian.

DOI
10.1063/1.5080623

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We investigate the transmission properties of Fabry–Pérot microcavities made of metal mirrors containing the organic dye molecule, generally called Lemke. We synthesized Lemke dye and fabricated the microcavities by using simple vacuum evaporation and spin-coating methods. The vacuum Rabi splitting energy increases in proportion to the square root of the absorption coefficient of the cavity layers and exceeds 1 eV at maximum. The ratio of the vacuum Rabi splitting energy to the matter transition energy reaches 0.42, so we consider that the ultrastrong-coupling regime was attained. The dispersion relation is reasonably interpreted by using the full Hopfield Hamiltonian.
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.
Summary form only given. Organic dye molecules have been used in great many scientific and technological applications. Among these, the polycyclic aromatic hydrocarbons (PAH) behave very favourably as quantum emitters when embedded in organic crystals at temperatures below 4K. PAHs can serve as solid-state emitters with remarkable optical properties such as near-unity quantum efficiency and high photostability. However, transitions to short-lived molecular vibrational levels reduce the scattering cross section by a branching ratio of about 30-50%. In order to overcome this shortcoming and render the molecule as a two-level system, one can enhance its zero-phonon emission by using the Purcell effect, e.g., via coupling to an optical cavity, to obtain a near-unity branching ratio. Here we report the first coherent coupling of a single molecule to a scannable, tunable and broadband microcavity. The cavity consists of a planar distributed Bragg reflector and a micromirror with a radius of curvature of 5 μm fabricated with focused ion-beam milling [1] and coated with silver. By integrating an organic matrix in the microcavity, we are able to coherently couple individual molecules to the cavity mode at liquid helium temperature.
Summary form only given. The interaction between light and matter can be significantly altered by placing the material in an optical microcavity. Under appropriate conditions strong coupling may occur, a process in which the confined electromagnetic field of the microcavity dramatically modifies the optical transitions of the material, resulting in an anti-crossing (Rabi splitting) of the coupled modes of the microcavity. Recently strong coupling has been observed in organic materials including J-aggregates of cyanine dyes. They have the desired properties of large oscillator strength and narrow linewidth, and have shown large Rabi splitting at room temperature. We report here significant strong coupling in a new structure, a metal clad organic microcavity.
We discuss the frequency dependence of the spontaneous-emission rate (power) in a Fabry-Perot microcavity containing a Lorentz dielectric, with emphasis on modifications of the spectrum under the circumstances of the strong medium-cavity coupling. With the standard-cavity tuning, the total spontaneous-emission power spectrum consists of a multiwave version of the familiar low-frequency vacuum Rabi split peak and a broad structure on the high-frequency side coming from the enhanced spontaneous emission into the continuum of the obliquely propagating waves. This form of the spectrum derives from the properties of the (single-wave) radiation-intensity spectrum of the molecule. Depending on the observation direction, the radiation-intensity spectrum exhibits either a double-peak structure characteristic of the vacuum Rabi splitting, as observed in light transmisssion and reflection experiments, or a single-peak structure describing the enhanced spontaneous emission at the corresponding cavity resonant frequency.
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.