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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Fluorescence of organic molecules in the microcavity at two-photon absorption

Elena E. Bykova, Аlexander А. Zemlyanov, Yu. É. Geints

Published Feb 14, 2006• 0 citations
Publisher

Abstract

The problem about fluorescence of organic molecules located in micropartical-cavity at two-photon absorption in the condition of laser pulse radiation influence taking into account stimulated transitions was theoretically investigated. The approach based on the metod of open-resonator theory with light fields expanded in series of quasinormal vibrational eigenmodes of a dielectric full sphere was used. For active molecules in microcavity the model of generalized two-level system noted with processes of two-photon absorption and emission, spontaneous and stimulated emissions on stokes frequencies was considered. The kinetic equations solution were obtained.

DOI
10.1117/12.675329

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The problem about fluorescence of organic molecules located in micropartical-cavity at two-photon absorption in the condition of laser pulse radiation influence taking into account stimulated transitions was theoretically investigated. The approach based on the metod of open-resonator theory with light fields expanded in series of quasinormal vibrational eigenmodes of a dielectric full sphere was used. For active molecules in microcavity the model of generalized two-level system noted with processes of two-photon absorption and emission, spontaneous and stimulated emissions on stokes frequencies was considered. The kinetic equations solution were obtained.
The problem about two-photon induced fluorescence of organic dye active molecules located in spherical transparent microparticles at the ultrashort laser pulses influence was theoretically investigated. The system of kinetic equations for laser generation was written taking into account stimulation transitions. Generation regimes of stimulated radiation were found. Resonator properties of spherical microparticles were theoretically investigated using the method of expanding optical fields into series of eigenfunctions. The breakdown of the beginning of stimulated radiation in the microparticle was determined. It was shown that stimulated radiation intensity depends on degree of its spatial overlap with all other modes of the pump radiation. The interpretation of experimental data of two-photon induced fluorescence in the particles with organic dye was carried out.
The problem about two-photon induced fluorescence of organic dye active molecules located in spherical transparent microparticles at the ultrashort laser pulses influence was theoretically investigated. The system of kinetic equations for laser generation was written taking into account stimulation transitions. Generation regimes of stimulated radiation were found. Resonator properties of spherical microparticles were theoretically investigated using the method of expanding optical fields into series of eigenfunctions. The breakdown of the beginning of stimulated radiation in the microparticle was determined. It was shown that stimulated radiation intensity depends on degree of its spatial overlap with all other modes of the pump radiation. The interpretation of experimental data of two-photon induced fluorescence in the particles with organic dye was carried out.
A calculation is made of the stimulated emission threshold of organic dye solutions as a function of the diffusion coefficient, intensity of induced singlet–singlet or triplet–triplet absorption at the stimulated emission wavelength, steepness of the leading edge of pump pulses, and other parameters. It is shown that, if the dipole moment of a fluorescence transition is perpendicular to the dipole moments of associated induced singlet–singlet or triplet–triplet absorption transitions, the laser threshold of high–viscosity solutions is considerably lower than that of low-viscosity systems. The maximum value of the ratio of the cross sections of the singlet-singlet absorption and stimulated emission, at which a given molecule ceases to emit stimulated radiation, increases from 1 to 3 when the rotational diffusion coefficient decreases from ∞ to 0.
The process of stimulated emission from two nearby microlasers excited in an active microscopic cavity has been adopted to investigate the onset of the Bose-Einstein correlation established over very short distances d of order λ from the fluorescence source of stimulated radiation.1,2 A marked effect of photon localization, which is unexpected according to standard QED, has been experimentally found. The effect is relevant for distances of the order bλ, for b ranging between 10 and 100, for a microcavity spacing equal to λ/2, i.e., in the cavity single resonant mode condition.2 The effect tends to disappear for macroscopic cavity spacings, reproducing in this case the expected QED behavior, i.e., the one which is well known in standard laser physics. The dependence of the effect on the microcavity finesse and on the mirror reflectivities has been investigated.
This work explores the feasibility of inducing lasing action in a single dye molecule using an optical microcavity. A single-molecule light source is proposed, in which a microcavity-coupled dye molecule is pumped by multiple energy donors via an intermolecular resonance energy transfer mechanism. A quantitative model based on realistic parameters for microcavities and for organic dyes shows that stimulated emission may become dominant over spontaneous fluorescence under optimal yet technically reachable conditions, suggesting the likelihood of achieving a single-molecule lasing photon source with the proposed device. Lasing of a single dye molecule generates signals much brighter than spontaneous fluorescence, and may find applications in a wide range of fields from physics and chemistry to biology.
We describe recent results of experiments probing single molecules in the surface of spherical microcavities. Effects of spatial photoselection have been recently observed through changes in the single-molecule fluorescence photon statistics. In addition to being a sensitive probe of the highly interesting boundary region between classical and quantum mechanics, cavity-modified spontaneous emission and the possibility of single-molecule stimulated emission hold exciting promise as a means of exceeding sensitivity limitations such as photobleaching and absorption saturation in single molecule fluorescence detection. Ongoing efforts such as fluorescence imaging of single molecules on the surface of microspheres and attempts to observe single- molecule stimulated emission will also be described.