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Lasing in strongly scattering dielectric microstructures

Lucia Florescu

Published Jan 1, 2004• 0 citations
OpenAlex

Abstract

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.

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Semiclassical theory of lasing in photonic crystals

Lucia Florescu, Kurt Busch, Sajeev John

We present a theoretical analysis of laser action within the bands of propagating modes of a photonic crystal. Using Bloch functions as carrier waves in conjunction with a multiscale analysis, we derive the generalized Maxwell–Bloch equations for an incoherently pumped atomic system in interaction with the electromagnetic reservoir of a photonic crystal. These general Maxwell–Bloch equations are similar to the conventional semiclassical laser equations but contain effective parameters that depend on the band structure of the linear photonic crystal. Through an investigation of steady-state laser behavior, we show that, near a photonic band edge, the rate of stimulated emission may be enhanced and the internal losses are reduced, which leads to an important lowering of the laser threshold. In addition, we find an increase of the laser output along with an additional narrowing of the linewidth at a photonic band edge.

Journal of the Optical Society of America B•Sep 1, 2002•70 citations

Theory of photon statistics and optical coherence in a multiple-scattering random-laser medium

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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.

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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.

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Theory of a one-atom laser in a photonic band-gap microchip

Lucia Florescu, Sajeev John, Tran Quang +1 more

We present a quantum theory of a coherently pumped two-level atom in a photonic band gap (PBG), coupled to both a multimode waveguide channel and a high-quality microcavity embedded within a photonic crystal. One mode is engineered to exhibit a sharp cutoff within the PBG, leading to a large discontinuity in the local photon density of states near the atom, and the cavity field mode is resonant with the central component of the Mollow spectrum of atomic resonance fluorescence. Another mode of the waveguide channel is used to propagate the pump beam. We derive analytical expressions for the optical amplitude, intensity, second-order correlation functions, and conjugate quadrature variances for the light emitted by the atom into the microcavity. The quantum degree of second-order coherence in the cavity field reveals enhanced, inversionless, nearly coherent light generation when the photon density of states jump between the Mollow spectral components is large. The cavity field characteristics are highly distinct from that of a corresponding high-$Q$ cavity in ordinary vacuum. In the case of a vanishing photon density of states on the lower Mollow sideband and no dipolar dephasing, the emitted photon statistics is Poissonian, and the cavity field exhibits quadrature coherence.

Physical Review A•Jan 26, 2004•43 citations

Resonant atomic switching near a photonic band-gap: Towards an all-optical micro-transistor

Marian Florescu A

In this thesis we demonstrate that the photonic band edge facilitates fundamental switching effects for resonant two-level atomic systems. In a photonic crystal, a coherent laser beam can drive a two-level atom to inverted atomic states, a phenomenon forbidden in ordinary vacuum. In this process, the atomic system switches from a passive medium to a gain medium as a function of the driving field intensity. We show that the large differential gain exhibited by the atomic medium is robust against non-radiative relaxation and dephasing mechanisms. This switching effect exhibits collective enhancement for a large number of two-level atoms within a cubic wavelength. In this case, the ensemble of atoms sharply switches to a highly inverted state at a very well defined threshold value of the laser field intensity. We next demonstrate that a probe laser field of prescribed wavelength experiences a substantial differential gain by slight modulations in the control laser field. We suggest that a doped photonic band gap material may, in this sense, be used as an all-optical micro-transistor. We analyze the effects of inhomogeneous line broadening on the probe beam spectrum and demonstrate that further electromagnetic density of states engineering combined with photo-bleaching techniques can be used to both offset the deleterious effects of inhomogeneous broadening and to enlarge the switching bandwidth. We investigate the prospects and challenges in designing microstructures with characteristics required by our proposal. We further show that the switching power and the response time of an all-optical transistor can be dramatically reduced by including collective effects, which also provide a natural mechanism of broadening of the gain spectrum. Finally, we develop an exact multi-photon scattering theory of resonance fluorescence in frequency-dependent photonic reservoirs. We show that, in the limit of weak driving field, the scattering cross section becomes strongly non-Lorentzian, reflecting the non exponential character of the atomic decay. As the driving field intensity increases, the scattered field acquires new features, consistent with predictions of a dynamical decoupling of the atomic system from the photonic reservoir.

•Jan 1, 2003•1 citation
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 present a theoretical analysis of laser action within the bands of propagating modes of a photonic crystal. Using Bloch functions as carrier waves in conjunction with a multiscale analysis, we derive the generalized Maxwell–Bloch equations for an incoherently pumped atomic system in interaction with the electromagnetic reservoir of a photonic crystal. These general Maxwell–Bloch equations are similar to the conventional semiclassical laser equations but contain effective parameters that depend on the band structure of the linear photonic crystal. Through an investigation of steady-state laser behavior, we show that, near a photonic band edge, the rate of stimulated emission may be enhanced and the internal losses are reduced, which leads to an important lowering of the laser threshold. In addition, we find an increase of the laser output along with an additional narrowing of the linewidth at a photonic band edge.
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.
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 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 present a quantum theory of a coherently pumped two-level atom in a photonic band gap (PBG), coupled to both a multimode waveguide channel and a high-quality microcavity embedded within a photonic crystal. One mode is engineered to exhibit a sharp cutoff within the PBG, leading to a large discontinuity in the local photon density of states near the atom, and the cavity field mode is resonant with the central component of the Mollow spectrum of atomic resonance fluorescence. Another mode of the waveguide channel is used to propagate the pump beam. We derive analytical expressions for the optical amplitude, intensity, second-order correlation functions, and conjugate quadrature variances for the light emitted by the atom into the microcavity. The quantum degree of second-order coherence in the cavity field reveals enhanced, inversionless, nearly coherent light generation when the photon density of states jump between the Mollow spectral components is large. The cavity field characteristics are highly distinct from that of a corresponding high-QQQ cavity in ordinary vacuum. In the case of a vanishing photon density of states on the lower Mollow sideband and no dipolar dephasing, the emitted photon statistics is Poissonian, and the cavity field exhibits quadrature coherence.
In this thesis we demonstrate that the photonic band edge facilitates fundamental switching effects for resonant two-level atomic systems. In a photonic crystal, a coherent laser beam can drive a two-level atom to inverted atomic states, a phenomenon forbidden in ordinary vacuum. In this process, the atomic system switches from a passive medium to a gain medium as a function of the driving field intensity. We show that the large differential gain exhibited by the atomic medium is robust against non-radiative relaxation and dephasing mechanisms. This switching effect exhibits collective enhancement for a large number of two-level atoms within a cubic wavelength. In this case, the ensemble of atoms sharply switches to a highly inverted state at a very well defined threshold value of the laser field intensity. We next demonstrate that a probe laser field of prescribed wavelength experiences a substantial differential gain by slight modulations in the control laser field. We suggest that a doped photonic band gap material may, in this sense, be used as an all-optical micro-transistor. We analyze the effects of inhomogeneous line broadening on the probe beam spectrum and demonstrate that further electromagnetic density of states engineering combined with photo-bleaching techniques can be used to both offset the deleterious effects of inhomogeneous broadening and to enlarge the switching bandwidth. We investigate the prospects and challenges in designing microstructures with characteristics required by our proposal. We further show that the switching power and the response time of an all-optical transistor can be dramatically reduced by including collective effects, which also provide a natural mechanism of broadening of the gain spectrum. Finally, we develop an exact multi-photon scattering theory of resonance fluorescence in frequency-dependent photonic reservoirs. We show that, in the limit of weak driving field, the scattering cross section becomes strongly non-Lorentzian, reflecting the non exponential character of the atomic decay. As the driving field intensity increases, the scattered field acquires new features, consistent with predictions of a dynamical decoupling of the atomic system from the photonic reservoir.