A semiclassical dynamic theory of the nonlinear propagation of a few interacting intense light pulses is applied to study the nonlinear counterpropagation of amplified spontaneous emission (ASE) induced by three-photon absorption of short intense laser pulses in a chromophore solution. Several important results from the modeling are reached for the ASE process developing in the regime of strong saturation. Accounting for ASE in both forward and backward directions with respect to the pump pulse results in a smaller efficiency of nonlinear conversion for the forward ASE compared with the case in which forward emission is considered alone, something that results from the partial repump of the absorbed energy to the backward ASE component; the overall efficiency is nevertheless higher than for the forward emission considered alone. The efficiency of nonlinear conversion of the pump energy to the counterpropagating ASE pulses is strongly dependent on the concentration of active molecules so that a particular combination of concentration versus cell length optimizes the conversion coefficient. Under certain specified conditions, the ASE effect is found to be oscillatory; the origin of oscillations is dynamical competition between stimulated emission and off-resonant absorption. This result can be considered one of the possible explanations of the temporal fluctuations of the forward ASE pulse [Nature 415, 767 (2002)].
A semiclassical dynamic theory of the nonlinear propagation of a few interacting intense light pulses is applied to study the nonlinear counterpropagation of amplified spontaneous emission (ASE) induced by three-photon absorption of short intense laser pulses in a chromophore solution. Several important results from the modeling are reached for the ASE process developing in the regime of strong saturation. Accounting for ASE in both forward and backward directions with respect to the pump pulse results in a smaller efficiency of nonlinear conversion for the forward ASE compared with the case in which forward emission is considered alone, something that results from the partial repump of the absorbed energy to the backward ASE component; the overall efficiency is nevertheless higher than for the forward emission considered alone. The efficiency of nonlinear conversion of the pump energy to the counterpropagating ASE pulses is strongly dependent on the concentration of active molecules so that a particular combination of concentration versus cell length optimizes the conversion coefficient. Under certain specified conditions, the ASE effect is found to be oscillatory; the origin of oscillations is dynamical competition between stimulated emission and off-resonant absorption. This result can be considered one of the possible explanations of the temporal fluctuations of the forward ASE pulse [Nature 415, 767 (2002)].
Competition between amplified spontaneous emission (ASE) and the four-wave-mixing (FWM) process has been observed under conditions of two-photon resonant excitation of the sodium 3d level. The nature of the competition is that the FWM process is able to prevent the occurrence of ASE, even though the gain of the ASE process calculated in the absence of competition effects is much larger than that of FWM. The ASE is suppressed because the fields generated by the FWM process create a new excitation pathway connecting the ground and 3d levels, and under quite general conditions this pathway interferes destructively with that due solely to the applied laser field. These effects are modeled theoretically by solving perturbatively the density-matrix equations of the atomic system, thereby determining the population in the upper level and the nonlinear polarization of the medium. The coupling between the various optical fields due to the nonlinear polarization is described by coupled amplitude equations. The solution to these equations predicts that when the wave-vector mismatch is not too large the fields evolve spatially to reach steady-state values, and that the population excited to the 3d level by the total steady-state optical field is much smaller than that due to the incident laser field alone. We have observed experimentally the suppression of ASE by FWM and have observed that this suppression does not occur when the medium is excited with counterpropagating beams that cannot efficiently excite the FWM process. In addition, we have conducted a series of experiments that shows that the degree of suppression of ASE depends on the intensity and focusing characteristics of the incident laser as expected on the basis of our theoretical model.
Competition has been observed between amplified spontaneous emission (ASE) and four-wave mixing (FWM). Previously, competition between an incoherent and coherent process was observed in the form of suppression of multiphoton ionization by third harmonic generation.1,2 In our experiment, an input laser was tuned precisely to the 3s → 3d two-photon allowed transition in atomic sodium vapor and the emission was observed in both the forward and backward directions. In these conditions, either FWM or ASE can occur. Ignoring the possibility of competition between these two processes, the calculated gain for ASE is much larger than that for FWM. However, we have observed experimentally that FWM and not ASE occur. To determine that it is the presence of efficient FWM that suppresses ASE, we have excited the atomic vapor instead with counterpropagating pump waves of different frequency. In this case, FWM, being a phase-matched process, cannot occur and strong ASE is observed. The nature of this competition is explained by solving the coupled Maxwell and density matrix equations for a three-level system. It is found that the suppression is due to the destructive interference between two different pathways of excitation of the 3d level which results in trapping of the population in the ground state.
The output of pulsed, homogeneously broadened amplified spontaneous emission (ASE) lasers operating under conditions of strong saturation is considered. An expression for the maximum power (energy) per unit volume that may be extracted from steady-state (pulsed) systems is derived and shown to be independent of the saturation intensity. Numerical calculations of the temporal evolution of the populations in the laser levels and the growth in the ASE fluence, peak intensity, and spectral width are presented for three types of laser system: quasi steady state, short pump pulses, and self-termination. In all cases the growth in the fluence of the ASE pulse is found to agree with an analytic solution derived for conditions of strong saturation. The calculated growth in intensity of the ASE pulse is compared with expressions derived by Pert [J. Opt. Soc. Am. B11, 1425 (1994)] for the steady-state case. As expected, good agreement is found for the quasi-steady-state system, but in the limit of strong saturation significant differences occur for the short pump pulse and self-terminating laser systems considered. For all cases considered, the variation of the spectral width of the ASE pulse is found to be in reasonable agreement with that predicted by Pert for steady-state conditions.
The coupling of forward and backward propagating waves is studied theoretically in the transition region between superfluorescence (SF) and amplified spontaneous emission (ASE). To accomplish this a computer code has been written that solves Maxwell's equations in time and two spatial dimensions and accounts for counter-propagation, diffraction, and temporal coherence in the Bloch equations. Diffraction is ignored in the present calculations. In the SF regime the coupling is generally weak, as found by others; however, I have found a randomly occurring shot-to-shot coupling that is quite significant in cases where one wave, forward or backward, becomes established from quantum noise first in the amplified rod. In this case the wave that arises second is strongly coupled to the first. In the ASE regime the propagation shows strong forward-backward coupling and the characteristic spatial profile of the inversion that tends to zero at either end and to the small signal value of one in the middle of the amplifier. In the transion region the propagation shows mixed SF and ASE behavior.
We report an observation of nonsaturable absorption of light. When a laser medium in a small aspect ratio geometry is uniformly and transversely pumped, amplified spontaneous emission (ASE) builds up along the longitudinal axis. The higher ASE intensity at the ends of the cell repopulates the ground state through the stimulated emission process more rapidly than at the center of the cell. Therefore, the absorption of the pump light is enhanced at the ends and the transmitted pump beam shows a nonuniform profile with a peak at the center. When the occupation of the states other than the upper lasing state and the ground state can be ignored, the normalized profile of the transmitted pump beam becomes identical to that of the fluorescence depicting the upper state population distribution. This fact has been confirmed experimentally with a R6G dye cell pumped with various intensities of frequency doubled Nd:YAG laser (λ = 532 nm, 10-ns pulse duration). The percentage of the absorbed pump energy at the ends of the cell remains the same, virtually nonsaturable, whereas at the center it decreases as the pump intensity increases.
Paraxial Maxwell-Bloch theory is used to describe amplified spontaneous emission (ASE) in strongly inverted media. Counterpropagation of waves coupled through gain saturation and diffraction, and pumping by a laser beam which propagates transverse to the amplifier are included in the treatment. The reactive part of the medium polarization is calculated by population-rate equations in the limit of rapid dephasing of the atomic dipoles. The spontaneous emission noise source needed for the numerical simulation of Maxwell's equations is derived from microscopic theory by coarse-graining, thereby establishing the compatibility of the spherically symmetric microscopic source with paraxial propagation theory. The three coupled Maxwell equations for the counterpropagating ASE waves and the transversely propagating pump wave are solved numerically in time and two spatial dimensions. This simulation is used to calculate the longitudinal profile of the transverse fluorescence, which measures the saturation of the gain, the longitudinal profile of the transmitted pump wave, which measures the saturation of pump absorption, and the transverse coherence function of the radiation emitted from the ends of the amplifier.