The effects of multifrequency-mode laser radiation on polarization-spectroscopy signal generation are investigated by direct numerical integration of the time-dependent density-matrix equations. The numerical solution of the density-matrix equations allows us to incorporate a physically reasonable model for pulsed dye-laser radiation in our analysis of the laser–resonance interaction. The laser radiation is modeled as the sum of electric fields from a finite number of modes that are assumed to have random pulse-to-pulse phases and exponentially distributed amplitudes. Calculations are performed for a homogeneously broadened resonance (only collisional broadening) and for a resonance that is both collision and Doppler broadened. The effect of the multimode laser radiation on polarization-spectroscopy line shapes and saturation curves is investigated for different values of the laser bandwidth and mode spacing and resonance collision and Doppler widths. The saturation parameter for the resonance is strongly dependent on the ratio of the laser bandwidth to the resonance collision width when the laser bandwidth is greater than the collision width. The pulse-to-pulse fluctuations in polarization-spectroscopy signal levels are found to decrease substantially for saturating pump intensities. The inclusion of the multimode laser structure into our density-matrix equations represents a significant advance in modeling the nonlinear interaction of laser radiation with atomic or molecular resonances.
© 2000 Optical Society of America
(020.2070) Atomic and molecular physics : Effects of collisions
(020.3690) Atomic and molecular physics : Line shapes and shifts
(120.1740) Instrumentation, measurement, and metrology : Combustion diagnostics
(270.2500) Quantum optics : Fluctuations, relaxations, and noise
(300.6390) Spectroscopy : Spectroscopy, molecular
William C. Giancola, Thomas A. Reichardt, and Robert P. Lucht, "Multi-axial-mode laser effects in polarization spectroscopy," J. Opt. Soc. Am. B 17, 1781-1794 (2000)