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Quantum Electronics and Laser Science Conference

Lasing in amplifying random media

Azriel Z. Genack, G. Berger, Michael Kempe, M. Larinov

Published Jun 7, 1996• 0 citations
OpenAlex

Abstract

Summary form only given. In this presentation we compute the emission properties from a colloidal suspension of titania particles in a Rhodamine 640 in methanol dye solution. Since feedback is negligible in these samples, wave interference is ignored in computing average transport within the medium. Consequently, the migration of pump and emitted photons is modeled as a random walk.

Related papers

Theory of lasing in a multiple-scattering medium

Sajeev John, Gen-Di Pang

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.

Physical Review A•Oct 1, 1996•190 citations

Spectral measurements of the emission from highly scattering gain media

G. Beckering, Stephan J. Zilker, D. Haarer

The spectral properties of the emission of a colloidal suspension of titanium dioxide particles in Rhodamine 640 perchlorate were studied systematically. The particle density rho, the dye concentration c, and the energy of the pump pulse were varied over several orders of magnitude; the dependence of the spectra on these three parameters is discussed. We discovered a strong correlation between the particle density and the dye concentration. The amplification by stimulated emission was found to be strongest when the absorption length l(a) and the mean-free-path length l(*) had approximately the same magnitude. The respective l(*) values were determined by a pulsed transmission experiment.

Optics Letters•Sep 15, 1997•42 citations

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We report enhanced emission and gain narrowing in Rhodamine 590 perchlorate dye in an aqueous suspension of polystyrene microspheres. A systematic experimental study of the threshold condition for and the gain narrowing of the stimulated emission over a wide range of dye concentrations and scatterer number densities showed several interesting features, even though the transport mean free path far exceeded the system size. The conventional diffusive-reactive approximation to radiative transfer in an inhomogeneously illuminated random amplifying medium, which is valid for a transport mean-free path much smaller than the system size, is clearly inapplicable here. We propose a new probabilistic approach for the present case of dense, random, weak scatterers involving the otherwise rare and ignorable sub-mean-free-path scatterings, now made effective by the high gain in the medium, which is consistent with experimentally observed features.

Applied Optics•Oct 20, 1997•39 citations

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The spatial and spectral evolution of emission from gain media with homogeneously distributed scatterers is modeled using a Monte Carlo simulation of the random walk of pump and emitted photons. We find a sharp transition to ultrafast, narrow-linewidth emission for a 10-ps incident pump pulse and a rapid approach to steady state for longer pulses. The threshold for this transition is raised significantly when the transverse diffusion of photons out of the excited region is substantial. The quantitative agreement of the results with recent observations of emission from random gain media lends further support to the interpretation of ``random lasers'' in terms of amplified spontaneous emission within a multiply-scattering medium.

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Light Propagation and Random Lasing

Regine Frank

In the last decade Anderson Localization of Light and Random Lasing has attracted a variety of interest in the community of condensed matter theory. The fact that a system so inartificial as a thin layer consisting of dust particles, which have amplifying properties, can produce coherent laser emission, is of a simple elegance, which promises new insights in fundamental physics. There is no need of an external feedback mechanism, like in the system of a conventional laser. Whereas several attempts try to enter the subject numerically by considering cavity approximations, this thesis is concerned with building a microscopically self-consistent theory of random lasing. Designing this method, we had to study light localization effects in random media including absorption and gain. Incorporating interference effects by means of Cooperon contributions we derived Anderson localized states for passive media. Mapping this on a system which consists of laser active Mie-scatterers in a passive medium, we found that by incorporation of the Cooperon, we loose the Anderson localization, but the system is weakly localized, which is sufficient for population inversion and stimulated emission.

•Jan 19, 2012•0 citations

Lasing in a random amplifying medium: Spatiotemporal characteristics and nonadiabatic atomic dynamics

Lucia Florescu, Sajeev John

We study the dynamics of lasing from photonic paints excited by short, localized, optical pulses, using a time-dependent diffusion model for light propagating in the medium containing active atoms. The full time-dependent, nonadiabatic nonlinear response of the atomic system to the local optical field intensity is described using the Einstein rate equations for absorption and emission of light. Solving the time-dependent diffusion equation for the light intensity in the medium with nonlinear gain and loss, we derive detailed information on the spectral, spatial, and temporal properties of the emitted laser light. Our model recaptures the effects of scatterers to narrow the emission spectral linewidth and to narrow the emitted pulse duration, at a specific threshold pump intensity. Our model also describes how this threshold pump intensity decreases with scatterer density and excitation spot diameter, in excellent agreement with experimental results.

Physical Review E•Sep 20, 2004•21 citations
Summary form only given. In this presentation we compute the emission properties from a colloidal suspension of titania particles in a Rhodamine 640 in methanol dye solution. Since feedback is negligible in these samples, wave interference is ignored in computing average transport within the medium. Consequently, the migration of pump and emitted photons is modeled as a random walk.
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.
The spectral properties of the emission of a colloidal suspension of titanium dioxide particles in Rhodamine 640 perchlorate were studied systematically. The particle density rho, the dye concentration c, and the energy of the pump pulse were varied over several orders of magnitude; the dependence of the spectra on these three parameters is discussed. We discovered a strong correlation between the particle density and the dye concentration. The amplification by stimulated emission was found to be strongest when the absorption length l(a) and the mean-free-path length l(*) had approximately the same magnitude. The respective l(*) values were determined by a pulsed transmission experiment.
We report enhanced emission and gain narrowing in Rhodamine 590 perchlorate dye in an aqueous suspension of polystyrene microspheres. A systematic experimental study of the threshold condition for and the gain narrowing of the stimulated emission over a wide range of dye concentrations and scatterer number densities showed several interesting features, even though the transport mean free path far exceeded the system size. The conventional diffusive-reactive approximation to radiative transfer in an inhomogeneously illuminated random amplifying medium, which is valid for a transport mean-free path much smaller than the system size, is clearly inapplicable here. We propose a new probabilistic approach for the present case of dense, random, weak scatterers involving the otherwise rare and ignorable sub-mean-free-path scatterings, now made effective by the high gain in the medium, which is consistent with experimentally observed features.
The spatial and spectral evolution of emission from gain media with homogeneously distributed scatterers is modeled using a Monte Carlo simulation of the random walk of pump and emitted photons. We find a sharp transition to ultrafast, narrow-linewidth emission for a 10-ps incident pump pulse and a rapid approach to steady state for longer pulses. The threshold for this transition is raised significantly when the transverse diffusion of photons out of the excited region is substantial. The quantitative agreement of the results with recent observations of emission from random gain media lends further support to the interpretation of ``random lasers'' in terms of amplified spontaneous emission within a multiply-scattering medium.
In the last decade Anderson Localization of Light and Random Lasing has attracted a variety of interest in the community of condensed matter theory. The fact that a system so inartificial as a thin layer consisting of dust particles, which have amplifying properties, can produce coherent laser emission, is of a simple elegance, which promises new insights in fundamental physics. There is no need of an external feedback mechanism, like in the system of a conventional laser. Whereas several attempts try to enter the subject numerically by considering cavity approximations, this thesis is concerned with building a microscopically self-consistent theory of random lasing. Designing this method, we had to study light localization effects in random media including absorption and gain. Incorporating interference effects by means of Cooperon contributions we derived Anderson localized states for passive media. Mapping this on a system which consists of laser active Mie-scatterers in a passive medium, we found that by incorporation of the Cooperon, we loose the Anderson localization, but the system is weakly localized, which is sufficient for population inversion and stimulated emission.
We study the dynamics of lasing from photonic paints excited by short, localized, optical pulses, using a time-dependent diffusion model for light propagating in the medium containing active atoms. The full time-dependent, nonadiabatic nonlinear response of the atomic system to the local optical field intensity is described using the Einstein rate equations for absorption and emission of light. Solving the time-dependent diffusion equation for the light intensity in the medium with nonlinear gain and loss, we derive detailed information on the spectral, spatial, and temporal properties of the emitted laser light. Our model recaptures the effects of scatterers to narrow the emission spectral linewidth and to narrow the emitted pulse duration, at a specific threshold pump intensity. Our model also describes how this threshold pump intensity decreases with scatterer density and excitation spot diameter, in excellent agreement with experimental results.