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Physica status solidi. C, Conferences and critical reviews/Physica status solidi. C, Current topics in solid state physics

Stimulated light emission in a dielectrically disordered composite porous matrix

E. Gross, Nicolei Künzner, Joachim Diener, Minoru Fujii, Victor Yu. Timoshenko, Dmitri I. Kovalev

Published Jun 1, 2005• 1 citation
Publisher

Abstract

We report on a medium exhibiting extremely efficient light scattering properties: a liquid network formed in a porous matrix. Liquid fragments confined in the solid matrix result in a random fluctuation of the dielectric function and act as scattering objects for photons. The optical scattering efficiency is defined by the filling factor of the liquid in the pores and its dielectric constant. The spectral dependence of the scattering length of photons indicates that the phenomenon is governed by a Mie-type scattering mechanism. The degree of the dielectric disorder of the medium, i.e. the level of opacity is tunable by the ambient vapor pressure of the dielectric substance. In the strongest scattering regime the scattering length of photons is found to be in the micrometer range. By incorporation of dye molecules in the voids of the porous layer a system exhibiting optical gain is realized. In the multiple scattering regime the optical path of diffusively propagating photons is enhanced and light amplification through stimulated emission occurs: a strong intensity enhancement of the dye emission accompanied by significant spectral narrowing is observed above the excitation threshold for a layer being in the opalescence state. (© 2005 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim)

DOI
10.1002/pssc.200461141

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We report on a medium exhibiting extremely efficient light scattering properties: a liquid network formed in a porous matrix. Liquid fragments confined in the solid matrix result in a random fluctuation of the dielectric function and act as scattering objects for photons. The optical scattering efficiency is defined by the filling factor of the liquid in the pores and its dielectric constant. The spectral dependence of the scattering length of photons indicates that the phenomenon is governed by a Mie-type scattering mechanism. The degree of the dielectric disorder of the medium, i.e. the level of opacity is tunable by the ambient vapor pressure of the dielectric substance. In the strongest scattering regime the scattering length of photons is found to be in the micrometer range. By incorporation of dye molecules in the voids of the porous layer a system exhibiting optical gain is realized. In the multiple scattering regime the optical path of diffusively propagating photons is enhanced and light amplification through stimulated emission occurs: a strong intensity enhancement of the dye emission accompanied by significant spectral narrowing is observed above the excitation threshold for a layer being in the opalescence state. (© 2005 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim)
We report on a medium exhibiting extremely efficient light scattering properties: a liquid network formed in a porous matrix. Liquid fragments confined in the solid matrix result in a random fluctuation of the dielectric function and act as scattering objects for photons. The optical scattering efficiency is defined by the filling factor of the liquid in the pores and its dielectric constant. The spectral dependence of the scattering length of photons indicates that the phenomenon is governed by a Mie-type scattering mechanism. The degree of the dielectric disorder of the medium, i.e. the level of opacity is tunable by the ambient vapor pressure of the dielectric substance. In the strongest scattering regime the scattering length of photons is found to be in the micrometer range. By incorporation of dye molecules in the voids of the porous layer a system exhibiting optical gain is realized. In the multiple scattering regime the optical path of diffusively propagating photons is enhanced and light amplification through stimulated emission occurs: a strong intensity enhancement of the dye emission accompanied by significant spectral narrowing is observed above the excitation threshold for a layer being in the opalescence state.
We report on light amplification through stimulated emission in a dielectrically disordered medium. Liquid fragments confined in the solid matrix of porous quartz layers result in a random fluctuation of the dielectric function, and dye molecules embedded in the voids yield optical gain. The level of opacity is tunable by the ambient vapor pressure of the dielectric substance. In the multiple scattering regime, a strong intensity enhancement of the dye emission accompanied by significant spectral narrowing is observed above the threshold for a layer being in the opalescence state.
In several recent experiments, isotropic lasing action was observed in paints that contain rhodamine 640 dye molecules in methanol solution as gain media and titania particles as optical scatterers. These so-called paint-on laser systems are extraordinary because they are highly disordered systems. The microscopic mechanism for laser activity and the coherence properties of light emission in this multiple-light-scattering medium have not yet been elucidated. In this paper we derive the emission intensity properties of a model dye system with excited singlet and triplet electronic energy levels, which is immersed in a multiple-scattering medium with transport mean free path l*. Using physically reasonable estimates for the absorption and emission cross section for the singlet and triplet manifolds, and the singlet-triplet intersystem crossing rate, we solve the nonlinear laser rate equations for the dye molecules. This leads to a diffusion equation for the light intensity in the medium with a nonlinear intensity-dependent gain coefficient. Using this model we are able to account for nearly all of the experimentally observed properties of laser paint reported so far when l*\ensuremath{\gg}${\ensuremath{\lambda}}_{0}$, the emission wavelength. This includes the dependence of the peak intensity of amplified emission on the mean free path l*, the dye concentration \ensuremath{\rho}, and the pump intensity characteristics. Our model recaptures the collapse of the emission linewidth at a specific threshold pump intensity and describes how this threshold intensity varies with l*. In addition, our model predicts a dramatic increase in the peak intensity and a further lowering of the lasing threshold for the strong scattering limit l*\ensuremath{\rightarrow}${\ensuremath{\lambda}}_{0}$. This suggests a striking enhancement of the characteristics of laser paint near the photon localization threshold in a disordered medium. \textcopyright{} 1996 The American Physical Society.
In the first part of this thesis, a detailed analysis of lasing in random multiple-light-scattering media with gain is presented. Random laser emission is analyzed using a time-dependent diffusion model for light propagating in the medium containing active atoms. We demonstrate the effects of scatterers to narrow the emission spectral linewidth and to shorten the emitted pulse duration at a specific threshold pump intensity. This threshold pump intensity decreases with scatterer density and excitation spot diameter, in excellent agreement with experimental results. The coherence properties of the random laser are studied using a generalized master equation. The random laser medium is treated as a collection of low quality-factor cavities, coupled by random photon diffusion. Laser-like coherence, on average, is demonstrated above a specific pumping threshold. We demonstrate that with stronger scattering, the pumping threshold for the transition from chaotic to isotropic coherent light emission decreases and enhanced optical coherence for the emitted light is achieved above threshold. The second part of this thesis presents a study of lasing in photonic crystals (PCs). The emission from an incoherently pumped atomic system in interaction with the electro-magnetic reservoir of a PC is analyzed using a set of generalized semiclassical Maxwell-Bloch equations. We demonstrate that the photonic band edge facilitates the enhancement of stimulated emission and the reduction of internal losses, leading to an important lowering of the laser threshold. In addition, an increase of the laser output at a photonic band edge is demonstrated. We next develop a detailed quantum theory of a coherently pumped two-level atom in a photonic band gap material, coupled to both a multi-mode wave-guide channel and a high-quality micro-cavity embedded within the PC. The cavity field characteristics are highly distinct from that of a corresponding high-Q cavity in ordinary vacuum. We demonstrate enhanced, inversionless, and nearly coherent light generation when the photon density of states (DOS) jump between the Mollow spectral components of atomic resonance fluorescence is large. In the case of a vanishing photon DOS on the lower Mollow sideband and no dipolar dephasing, the emitted photon statistics is Poissonian and the cavity field exhibits quadrature coherence.
We predict the coexistence and competition of random lasing and stimulated Raman scattering (SRS) in active disordered random media. We develop a simple model that includes both mechanisms coupled to diffusion equation. We find that the prevalence of a nonlinear mechanism over the other is determined by the degree of scattering. This is confirmed experimentally in dye-infiltrated three-dimensional porous silica-based disordered samples, with controllable pore size and transport properties. Experimentally, random lasing dominates in a sample with a large transport mean free path, l t ≈ 100 μm, while it gives way to SRS for l t ≈ 25 μm. The competition is explained in terms of disorder-dependent pump depletion and fluorescence saturation.
We report on random lasing from a dye-scatterer system directly excited by evanescent modes formed over a dielectric-dielectric interface. The system is quasi-two-dimensional because of the subwavelength exponential decay of the excitation energy. Spectral narrowing by a factor of approximately 13 was obtained under diffusive scattering conditions. The peak intensity exhibited a unique dual-saturation behavior due to the localized nature of the excitation. We observed a reduction of threshold for samples with a higher dye concentration because of a larger excitation-state occupation number within the same interaction volume.