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Physical Review A

Fluorescence lifetimes of molecular dye ensembles near interfaces

Norbert Danz, Jörg Heber, Andreas Bräuer, Richard M. Kowarschik

Published Dec 26, 2002• 29 citations
Publisher

Abstract

Fluorescence lifetimes of thin, rhodamine 6G-doped polymer layers in front of a mirror have been determined as a function of the emitter-mirror separation and the conditions of excitation and observation. Lifetime is well known to depend on the spatial emitter-mirror separation. The explanation of experimental data needs to consider direction, polarization, and numerical aperture of the experimental system. As predicted theoretically, experimental results depend on the conditions of illumination and observation, because of the different lifetimes of emitters aligned horizontally or vertically with respect to the plane of interfaces and their selection by the experimental system. This effect is not observable when ions are used as a source of fluorescence, because ensemble averaging depends on the properties of sources.

DOI
10.1103/physreva.66.063809

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Fluorescence lifetimes of thin, rhodamine 6G-doped polymer layers in front of a mirror have been determined as a function of the emitter-mirror separation and the conditions of excitation and observation. Lifetime is well known to depend on the spatial emitter-mirror separation. The explanation of experimental data needs to consider direction, polarization, and numerical aperture of the experimental system. As predicted theoretically, experimental results depend on the conditions of illumination and observation, because of the different lifetimes of emitters aligned horizontally or vertically with respect to the plane of interfaces and their selection by the experimental system. This effect is not observable when ions are used as a source of fluorescence, because ensemble averaging depends on the properties of sources.
We have studied spectra and angular distribution of emission in Fabry–Perot cavities formed by two silver mirrors separated by a layer of poly (methyl methacrylate) polymer doped with rhodamine 6G (R6G) dye in low ( 20 g / l ) and high ( 200 g / l ) concentrations. The frequency of emission radiated to a cavity mode was larger at large outcoupling angles—the “rainbow” effect. At the same time, the angle of the strongest emission was also determined by the cavity size: the larger the cavity, the larger the angle. The angular distribution of emission is commonly dominated by two symmetrical lobes (located at the intersection of the three-dimensional emission cone with a horizontal plane) pointing to the left and to the right of the normal to the sample. Despite the strong Stokes shift in R6G dye, the branch of the cavity dispersion curve obtained in the emission experiment is positioned above the one obtained in the reflection (extinction) experiment. Some dye molecules are poorly coupled to cavity modes. Their emission has very broad angular distribution with the maximum at θ = 0 ∘ . The signatures of strong cavity–exciton coupling were observed at high dye concentration ( 200 g / l ) but not at low concentration ( 20 g / l ). The evidence of the effect of strong coupling on emission is exemplified by a strong difference in the angular distribution of emission in two almost identical cavities, one with and another without strong coupling. Most importantly, we have demonstrated the possibility to control the ground state concentration, the coupling strength, and the dye emission spectra with Q-switched laser pulses.
The spontaneous-emission rates of emitters embedded in a thin layer 0 of a loss-free dielectric depend on their optical environment, i.e., on the optical properties of the two media 1 and 2 adjoining layer 0. For electric- and magnetic-dipole transitions the spontaneous-emission rates, normalized with respect to those in an infinite medium 0, are expressed in terms of the Fresnel reflection coefficients for plane and evanescent waves incident from medium 0 on the interfaces to the planar-stratified or homogeneous media 1 and 2, respectively. From this result which is valid for arbitrary layer thicknesses d0{d}_{0}d0​ we derive an approximation for extremely thin layers of optical thickness ${n}_{0}{d}_{0}\ensuremath{\ll}\frac{\ensuremath{\lambda}}{8}$ (where $\ensuremath{\lambda}$ is the emission wavelength) between two homogeneous loss-free dielectric media 1 and 2. For the normalized spontaneous-emission rates as functions of the refractive indices nj{n}_{j}nj​ of media j=0,1,and2j=0, 1, \mathrm{and} 2j=0,1,and2 analytical expressions are obtained. We have used these expressions previously without proof [Phys. Rev. B 21, 4814 (1980)] to analyze experimentally observed changes in the fluorescence lifetime of Eu3+{\mathrm{Eu}}^{3+}Eu3+ ions in varying optical environments, which yielded the quantum efficiency of the emitting state.
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.