We report the theoretical analysis for tuning the quantum efficiency of solid state random lasers. Vollhardt-Wölfle theory of photonic transport in disordered non-conserving and open random media, is coupled to lasing dynamics and solved positionally dependent. The interplay of non-linearity and homogeneous non-radiative frequency conversion by means of a Stokes-shift leads to a reduction of the quantum efficiency of the random laser. At the threshold a strong decrease of the spot-size in the stationary state is found due to the increase of non-radiative losses. The coherently emitted photon number per unit of modal surface is also strongly reduced. This result allows for the conclusion that Stokes-shifts are not sufficient to explain confined and extended mode regimes.
We report the theoretical analysis for tuning the quantum efficiency of solid state random lasers. Vollhardt-Wölfle theory of photonic transport in disordered non-conserving and open random media, is coupled to lasing dynamics and solved positionally dependent. The interplay of non-linearity and homogeneous non-radiative frequency conversion by means of a Stokes-shift leads to a reduction of the quantum efficiency of the random laser. At the threshold a strong decrease of the spot-size in the stationary state is found due to the increase of non-radiative losses. The coherently emitted photon number per unit of modal surface is also strongly reduced. This result allows for the conclusion that Stokes-shifts are not sufficient to explain confined and extended mode regimes.
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 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.
Light propagation in matter is described by vibration eigenstates, called modes, which characterize the light-matter interaction. In the specific case of random media, according to the strength of the disorder, the modes can be either extended over the whole system or spatially localized. This disorder-based confinement is called Anderson’s localization.In the first part, we introduce basic notions used along this manuscript. In particular the light-matter interaction requires a semiclassical approach: The electromagnetic field is described by Maxwell’s equations while the quantum nature of matter must be considered. In this thesis open media are studied. In such systems the modal description requires a specific analytic treatment different from closed problems. In the second part, we focus on Anderson-localized modes in open passive random media. Any change of the disorder induces modifications of modes. Therefore, it enables the control over the light properties. Moreover, when inserting an emitter inside an Anderson-localized mode, strong light-matter interaction regimes can be reached. In the third part, active random media, commonly called random lasers, are introduced. Using our experimental achievements, characteristics of random lasers are presented. The notion of mode enables us to describe complex mechanisms involved in the lasing emission. Last, we demonstrate both experimentally and numerically that a non-uniform excitation of random lasers can lead to a control of the properties of the emission. In particular a multimode spectrum for a uniform pumping can be turned into single-mode using an adapted pumping.
We investigated several types of random lasing modes against frequency and the excitation of active medium. Random lasing occurring from multiple light scatterings and the interference effect of the scattered light has various complex lasing states in disordered structures, in which light waves are localized in various forms. Modes of random lasing are generally classified into localized, extended and transition modes based on their localization types. Numerical methods are used for analysing such complex phenomena. In this paper, a finite-element method is used to investigate the relationship among lasing modes, frequency and population inversion density of active medium for random lasing. Light amplification defined as the ratio of radiative powers between excited and non-excited states of the active medium is computed by changing both the frequency and the population inversion density of the active medium, which is modelled by the negative imaginary part of relative permittivity. The distributions of random lasing modes is strongly influenced by the lasing frequency. We also found that the localized modes that are strongly confined lasing modes in disordered structures do not appear in the frequency ranges in which mean free paths are approximately equal to the half-wavelength.
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 any quantum or wave system dissipation leads to decoherence. Therefore, it was surprising in first instance when experiments on strongly lossy random lasers showed unambiguously by measurements of the photon statistics and of the lasing mode volume that coherent feedback is possible in such systems3-5,8. In coherent-feedback lasers the photons form a far-from-equilibrium condensate in the sense that a single quantum state is occupied by a macroscopic number of photons15. We demonstrate that the lossy dynamics of random lasers alone imply a three dimensional finite lasing mode extent, thus resolving the puzzle about coherent feedback without resonator. Our theory of random lasing including nonlinear gain and gain saturation predicts a characteristic dependence of this lasing mode volume on the pump intensity, which can be tested experimentally.