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International Conference on Transparent Optical Networks

A scanning fiber-based microcavity for controlling single molecule emission

Costanza Toninelli, Y. L. Delley, Thilo Stöferle, Alois Renn, Stephan Götzinger, Vahid Sandoghdar

Published Jun 1, 2010• 0 citations
Publisher

Abstract

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.

DOI
10.1109/icton.2010.5549008

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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.
Optical microcavities are structures which confine light to a small region in the range of one wavelength. The radiation of a quantum emitter is coupled to cavity resonances which leads to an optical confinement of the broadband fluorescence. A practical design for this single-mode microcavity is formed by two silver mirrors enclosing a transparent dielectric medium with single quantum emitters. Steiner et al. have shown that the fluorescence spectra and decay lifetimes of single molecules in this Fabry-Perot type microcavity are strongly dependent on the resonator length.
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.
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.
Small optical microresonators are structures which confine light to volumes with dimensions on the order of one wavelength and provide an important means for controlling light-matter interaction in integrated optics. In this Paper, we would like to present our work on the study of the interaction of single quantum emitters or nanoparticles located in the confined optical field of a single-mode microresonator. The interaction possibilities between a general photonic system and a quantum system are discussed, with special focus on the effect of resonant microcavities. For the case of the optical microresonator used in our experiments, we present a model based on the transfer matrix method which can analytically describe the radiative enhancement of even complex resonator geometries. This allows not only the optimization of resonator geometries, but gives accurate information on the radiative processes occurring in the cavity, allowing the extraction of information normally inaccessible in optical measurements.
The interaction between light and matter has attracted much attention not only for fundamental research but also for applications. The open Fabry-Perot cavity provides an excellent platform for such a study due to strong optical confinement, spectral and spatial and tunability, and the feasibility of optical fiber integration. In this review, first, the basic properties of open Fabry-Perot cavities and the fabrication techniques are introduced. Then recent progress of weak coupling, strong coupling and bad emitter regimes is discussed. Finally, the challenges to and perspectives in this respect are presented.