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Physical Review E

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

Lucia Florescu, Sajeev John

Published Sep 20, 2004• 21 citations
Publisher

Abstract

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.

DOI
10.1103/physreve.70.036607

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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.
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.
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 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.
We derive the photon-number probability distribution and the resulting degree of second-order optical coherence for light emission from a uniformly distributed active species within a multiple-light-scattering medium. This is obtained from a master equation describing the probability distribution for photons in the vicinity of position r, traveling with a wave vector k, related, in turn, to a coarse-grained average of the optical Wigner coherence function. Using a simple model for isotropic, spatially uncorrelated scatterers, this reduces to a generalization of the master equation of a conventional laser in which the medium behaves like a random collection of low-quality factor cavities that are coupled by photon diffusion between a given cavity and its neighbors. Laserlike coherence, on average, is obtained in the random laser above a specific pumping threshold. Photon-number statistics above and below the lasing threshold are computed by first assuming that the atomic response to the local electromagnetic fields is nearly instantaneous. Corrections to this simple model, arising from nonadiabatic atomic dynamics, are then estimated. The dependence of the photon statistics on scatterer density, gain concentration, and position within a sample reveal that, on average, increase of the scattering strength (decrease of the photon transport mean free path) in the medium leads to a sharper peak in the local photon-number distribution, characteristic of increased local coherence in the optical field. We also evaluate the coherence of the output field at points outside the random-laser medium. This is a weighted average of radiation emitted at different positions in the sample, exhibiting varying degrees of coherence due to variations in the local pumping intensity.
In two recent works, the authors have investigated the spectro-temporal properties of the random laser emission from solid state dye-doped powders in picosecond pumping regime. Each emission pulse consists, both above and below threshold, in a collection of narrow peaks of a spectro-temporal width at the theoretical limit (ΔωΔt≅1). The distribution of path lengths traveled inside the diffusive active medium by photons that can be amplified by stimulated emission explains this behavior, as demonstrated by a simple theoretical model developed by the authors. The aim of the present work is, first, to develop an implemented model that does not depend on fitting parameters, and which is compatible with the energetic and spectro-temporal properties of the material; and second, to get knowledge about the spatial properties of the emission. The transverse coherence size of each emitted photon packet has been measured; and in addition, we have shown the existence of spatial fluctuations of the emission of these materials, as our model predicts.
The spatial formation of coherent random laser modes in strongly scattering disordered random media is a central feature in the understanding of the physics of random lasers. We derive a quantum field theoretical method for random lasing in disordered samples of complex amplifying Mie resonators which is able to provide self-consistently and free of any fit parameter the full set of transport characteristics at and above the laser phase transition. The coherence length and the correlation volume respectively is derived as an experimentally measurable scale of the phase transition at the laser threshold. We find that the process of stimulated emission in extended disordered arrangements of active Mie resonators is ultimately connected to time-reversal symmetric multiple scattering in the sense of photonic transport while the diffusion coefficient is finite. A power law is found for the random laser mode diameters in stationary state with increasing pump intensity.