Excited-state enhancement of third-order optical nonlinearities: photodynamics and characterization.

Based on the simplified five-level rate-equation theory, we investigate the hybrid third-order optical nonlinear processes which combine the instantaneous nonlinearity and the one-photon absorption induced excited-state nonlinearity. We obtain the analytical third-order nonlinear absorption and refraction coefficients originating from the singlet and triplet excited-state effects. We explore the photodynamic process and give the corresponding level diagram in the nanosecond, picosecond, and femtosecond regimes. We develop the pulse-duration-dependent Z-scan theory for characterizing the simultaneous instantaneous nonlinearity and cumulative effect of the excited-state nonlinearity. We also demonstrate the validity of the presented theory to analyze the experimental results.