The coherent properties of the temporally and spectrally narrowed emission of laser-induced fluorescence of organic dyes hosted inside artificial scattering matrices (random lasers) were investigated. The excitation source was a frequency-doubled 200-fs pulsed laser emitting at 400 nm. Spectral and temporal features were simultaneously recorded with a spectrograph and a streak camera operating in photon-counting mode. Photon-number distributions were thus created. The temporal coherence of the laserlike emission above and below the excitation energy threshold was investigated from the photon-number distribution that was obtained.
The coherent properties of the temporally and spectrally narrowed emission of laser-induced fluorescence of organic dyes hosted inside artificial scattering matrices (random lasers) were investigated. The excitation source was a frequency-doubled 200-fs pulsed laser emitting at 400 nm. Spectral and temporal features were simultaneously recorded with a spectrograph and a streak camera operating in photon-counting mode. Photon-number distributions were thus created. The temporal coherence of the laserlike emission above and below the excitation energy threshold was investigated from the photon-number distribution that was obtained.
In this work, the spectral and temporal properties of the random laser emission from dye-doped solid state powders are investigated in picosecond pumping regime. Ultrafast time-resolved spectroscopy achieved with a streak-camera has been used to perform a detailed study of the temporal evolution of the spectrum of their single pulses. Under conditions of low population inversion density, it is observed that the detected radiation occurs as isolated peaks with a very narrow spectro-temporally spread (ΔωΔt≅1). This behavior remains under conditions of high population inversion density, suggesting that the underlying physical mechanism that produces the emission is the same whatever the pumping conditions. Measurements carried out by varying the numerical aperture of the detection system show that each detected peak within a single pulse is associated with a photon pack emitted in a random direction and wavelength. The relationship between the distribution of paths lengths done by photons inside the active medium, and the gain explains the observed behavior.
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.
Regular and random lasing properties in a multiphoton active and highly scattering dye solution containing polystyrene microspheres of 366-nm diameter have been experimentally studied. Using 100-fs laser pulses of wavelength 790 nm and 1300 nm as the two- and three-photon excitation sources, the frequency-upconversion regular lasing of ~610 nm wavelength can be generated along both the forward and backward directions, characterized by high directionality, higher spectral intensity, and remarkable spectral narrowing. In the meantime, the random lasing can also be observed along all other directions, characterized by only spectral narrowing but with much lower spectral brightness. The spectral brightness ratio between the forward regular lasing and the random lasing is (104-105):1. Comparing to the input pump beam of ~3 mm diameter and divergence angle ofθ0≈0.9mrad, the forward lasing beam size and divergence angle were ~7 mm and ~(3-4)θ0, whereas the corresponding parameters were ~5 mm and∼1.5θ0for the backward lasing beam, indicating the phase-conjugation property of the latter.
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.
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.
We report measurement of the photon-counting distributions of nanosecond-duration light pulses. Photon counting is performed on light sources with widely different photon statistics, such as (1) a Q-switched Nd:YAG-laserpumped dye laser operating well above threshold and producing single-mode nanosecond pulses, (2) the same laser operating close to threshold, and (3) a rotating ground-glass aberrator illuminated by the laser pulses of case (1). The method is particularly suitable for the investigation of the statistics of light generated by the nonlinear interaction of radiation with matter.