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Conference on Lasers and Electro-Optics

3-D Orientation of Single Molecules in an Optical ?/2-Microresonator

Raphael Gutbrod, Alexey I. Chizhik, Dmitry Khoptyar, Anna M. Chizhik, Sebastian Bär, Alfred Johann Meixner

Published Jan 1, 2010• 0 citations
Publisher

Abstract

We present here a tunable microresonator which can be used to modify the optical properties of single quantum emitters. The 3D-orientation and position of a single molecule is determined with a radially polarized laser beam.
DOI
10.1364/qels.2010.qthl6

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Optical detection of molecules can often be challenging due to the lack of a closed cycling transition. In this paper, the authors explore the use of high-QQQ cavities and microresonators to increase the interaction time of light with a single molecule. Their technique could potentially also be applied for atoms or other quantum emitters.
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.
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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.