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IEEE Journal of Quantum Electronics

Effect of the solvent viscosity on the local irregular intensity fluctuations in high Fresnel number dye lasers

Óscar G. Calderón, I. Leyva, J.M. Guerra

Published Jan 1, 1999• 6 citations

Abstract

We study the influence of the solvent viscosity in the local irregular intensity fluctuations characteristic of high Fresnel number dye lasers. The relative amplitude of the fluctuations in a flashlamp-pumped dye laser is analyzed, We complete our previous work by using several solvents and different excitation energies above threshold. A decrease of the relative fluctuation amplitude is found as the solvent viscosity or the pumping energy increases. This effect is theoretically analyzed in the framework of the semiclassical Maxwell-Bloch equations, with a model based on the orientation of the dye molecules driven by the laser field in the solvent. These results point out the importance of the orientation of the dye molecules in the intensity fluctuation phenomenon.

DOI: 10.1109/3.737611

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We study the influence of the solvent viscosity in the local irregular intensity fluctuations characteristic of high Fresnel number dye lasers. The relative amplitude of the fluctuations in a flashlamp-pumped dye laser is analyzed, We complete our previous work by using several solvents and different excitation energies above threshold. A decrease of the relative fluctuation amplitude is found as the solvent viscosity or the pumping energy increases. This effect is theoretically analyzed in the framework of the semiclassical Maxwell-Bloch equations, with a model based on the orientation of the dye molecules driven by the laser field in the solvent. These results point out the importance of the orientation of the dye molecules in the intensity fluctuation phenomenon.

The behavior of the degree of polarization of the fluorescence and transmission versus intensity of complex molecules in high-viscosity solvents has been studied. We show that, in the usual case, when the electronic transition can be represented as a linear oscillator, molecules excited at low field have an anisotropic distribution; then, at high field, the distribution becomes isotropic. So, the relation between the transmission of the solution with intensity differs significantly from the transmission versus intensity relation derived by using the mean value of the cross section.

We examine from first principles the effects of a stochastic pump on the output fluctuations of a laser. The Hamiltonian for a four-level molecule interacting with a stochastic semiclassical pump field and quantized laser field is used to obtain density-matrix equations of motion. Noise from the pump field and from spontaneous emission is introduced systematically, as opposed to the ad hoc inclusion of random forces in the semiclassical equations. The relationship of this theory with previous quantum and semiclassical equations is described. New equations are derived on which computer simulations are performed to compare our theoretical results to experimental data for a single-mode dye laser.

We have studied the intensity fluctuations from a pulsed single-mode grazing incidence dye laser. The laser operates using rhodamine 6G dye pumped by 308-nm radiation from a XeCl excimer laser. Pump laser pulse duration is 6-8 ns and dye laser pulse duration is 2-3 ns. The spectral purity of the dye laser radiation is within 20% of the Fourier transform limit. Using event-mode recording involving the monitoring of pump laser intensity and dye laser intensity, we have determined the amplitude distribution from the dye laser at pumping conditions below, slightly above, and significantly above threshold. The amplitude fluctuations from the dye laser are well characterized by a Fokker-Planck model and they appear to be quantum in origin.

Recent theoretical analyses of the single-mode laser with colored-noise pump fluctuations have allowed the detailed prediction of the short-time behavior of the intensity autocorrelations of such a laser. In particular, a rounding off of the intensity correlation function on the time scale of the correlation time of the pump fluctuations has been predicted. We present results from experiments performed on a single-mode dye-laser system that clearly confirm these predictions. Numerical simulations of the laser Langevin equations including the colored-noise pump fluctuations are used to fit the experimental results.