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Single Molecules

Spontaneous Emission Control with Planar Dielectric Structures: An Asset for Ultrasensitive Fluorescence Analysis

C. Begon, Hervé Rigneault, Per Jonsson, John Rarity

Published Sep 1, 2000• 12 citations
Publisher

Abstract

We report on the interest of spontaneous emission control with planar dielectric multi-layer structures to increase the fluorescence collection efficiency in single-molecule detection experiments and ultrasensitive analysis. The effect of a very simple Fabry Perot microcavity on the radiation pattern of Eu3+ chelate molecules is introduced and discussed. Then the fluorescence correlation spectroscopy (FCS) technique is used to detect Cyanine 5 molecules on a simple mirror and Rhodamine 6G (R6G) molecules in a microcavity, both in liquid solutions. The respective advantages of those dielectric structures for increasing the count rate per molecule are described. The detection enhancement is used to demonstrate photon antibunching on the nanosecond time scale with a dilute solution of R6G molecules (10-9 M) in the microcavity.

DOI
10.1002/1438-5171(200009)1:3<207::aid-simo207>3.0.co;2-o

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We report on the interest of spontaneous emission control with planar dielectric multi-layer structures to increase the fluorescence collection efficiency in single-molecule detection experiments and ultrasensitive analysis. The effect of a very simple Fabry Perot microcavity on the radiation pattern of Eu3+ chelate molecules is introduced and discussed. Then the fluorescence correlation spectroscopy (FCS) technique is used to detect Cyanine 5 molecules on a simple mirror and Rhodamine 6G (R6G) molecules in a microcavity, both in liquid solutions. The respective advantages of those dielectric structures for increasing the count rate per molecule are described. The detection enhancement is used to demonstrate photon antibunching on the nanosecond time scale with a dilute solution of R6G molecules (10-9 M) in the microcavity.
A significant limitation in the detection and spectroscopy of individual dye molecules in liquid room temperature samples is the loss of fluorescence signal through chromophore photobleaching. Although often considered a fundamental restriction on sensitivity, it has been shown that the probability per excitation cycle of photobleaching may be reduced by enhancing the spontaneous emission rate of the chromophore located inside a microdroplet, which acts as a optical cavity. Studies of glycerol microdroplets containing R6G dye molecules, and levitated in a three-dimensional electrodynamic trap, have demonstrated a significant enhancement of both the fluorescence decay rate [1] and the total fluorescence yield [2] of the chromophore. Modification of the emission rate is greatest for molecules located near the surface of small (< 10 μm) microdroplets, where the influence of the droplet cavity modes of the droplet is most significant. To exploit this surface sensitivity, surfactant forms of rhodamine dyes were recently studied [3]. Fluorescence emission of the dye molecules, constrained to the droplet surface and with fixed transition moments perpendicular to the surface normal, were shown to be significantly enhanced at small droplet sizes. Additionally, at larger droplet sizes corresponding to higher droplet Q’s, preferential emission into the cavity modes was observed, however the detection of fluorescence photons was delayed by the storage time of the cavity, which may be on the same order as the fluorescence lifetime. These measurements, performed on relatively concentrated dye solutions, suggest that microcavity effects may be exploited to greatly enhance single molecule detection sensitivity in glycerol microdroplets. Furthermore, the large cavity storage time of the high-Q droplets opens the possibility for re-excitation of the molecule following emission into the droplet resonance, and subsequent stimulated emission, that is, single-molecule lasing.
A complete set of cavity modes in planar dielectric microcavities is presented which naturally includes guided modes. We show that most of these orthonormal fields can be derived from a coherent superposition of plane waves incoming on the stack from the air and from the substrate. Spontaneous emission of a dipole located inside the microcavity is analyzed, in terms of cavity modes. Derivation of the radiation pattern in the air and in the substrate is presented. The power emitted into the guided modes is also determined. Finally, a numerical analysis of the radiative properties of an erbium atom located in a Fabry-P\'erot multilayer dielectric microcavity is investigated. We show that a large amount of light is emitted into the guided modes of the structure, in spite of the Fabry-P\'erot resonance, which increases the spontaneous emission rate in a normal direction. \textcopyright{} 1996 The American Physical Society.
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.
We investigate theoretically and experimentally the optical properties of planar Ta2O5/SiO2 multilayer structures implanted with rare earth ions such as erbium and praseodymium. We demonstrate that the spontaneous emission can be strongly enhanced in a direction normal to the layers if the luminescent ions are located in the spacer of a resonant Fabry-Perot type microcavity. Nevertheless, we show that a large amount of light is emitted into the guided modes of the planar stack reducing the optical confinement which is likely to be reached within this type of dielectric microcavities.
The spontaneous emission from a thin layer of a dilute solution of fluorescent dye molecules within an optical microcavity has been studied. Strong fluctuations in fluorescence intensity are observed when the average number of molecules in the measurement volume is small. We have performed experiments that simultaneously characterize these fluctuations over nine orders of magnitude of time, from ns to s. These measurements have identified photon antibunching characteristic of single-molecule emission, along with triplet-state shelving and diffusion driven number fluctuations. The results give fundamental information on the kinetics of dye molecules and allow one to speculate about the prospect of using single molecules as sources of single photons for quantum optics.
We present both theoretical and experimental results on fluorescence of single defect centers in diamond nanocrystals embedded in a planar dielectric microcavity. From a theoretical point of view, we show that the overall fluorescence collection efficiency using moderate numerical aperture microscope objective can be enhanced by using a low quality factor microcavity. This could be used in particular for low temperature applications where the numerical aperture of collection microscope objectives is limited due to the experimental constraints. We experimentally investigate the control of the fluorescence spectrum of the emitted light from a single center. We show the simultaneous narrowing of the room temperature broadband emission spectrum and the increase of the fluorescence spectral density.