Nonlinear absorption of light: Optical saturation of electronic transitions in organic molecules with high intensity laser radiation

A review of spectroscopic properties of complex molecules is presented and used to show that a simple two-level scheme is inadequate to describe the optical bleaching of dye molecules. Experimental data are reported for the transmission of intense ruby laser radiation by several types of dyes. Rate equation analyses are carried out using steady-state solutions and iterative computer solutions; calculated bleaching curves are compared with our data for cryptocyanine. On these bases, we show that, in general, the optical bleaching process involves the removal of ground-state molecules to other states having smaller absorption cross sections at the exciting frequency, and that recovery of absorption at this frequency is characterized by a complex relaxation mechanism.