Polarization characteristics of nonlinear transmission in rigidly held saturable-dye molecules with random orientations

Polarization-dependent nonlinear transmissions are investigated by a pump-probe method in saturable-dye-doped films in which optically anisotropic saturable dyes are rigidly held with random orientations. The nonlinear transmissions measured by using uranine-doped poly(vinyl alcohol) films are compared with the theoretical predictions that are obtained by considering the effects of pump propagation and molecular orientation on the basis of a rate equation analysis for a four-energy-level model including an excited-state absorption. The measurements were conducted for the two cases of polarization states for which the polarization direction of the probe wave is either parallel or perpendicular to that of the pump wave; the experimental results considerably deviated from the theoretical ones for the probe wave perpendicularly polarized to the pump wave. It is shown that this is explained by modifying the energy level model to include the existence of a nearly-orthogonal component of the transition dipole moment associated with the ground-state absorption in uranine dyes.