Effects of excited-state absorption on two-photon absorbing materials

Many chromophores with a large two-photon absorptive cross section are hybrid materials where the two-photon absorption (TPA) is coupled to an excited-state absorption (ESA). We develop a numerical technique to investigate hybrid two-photon processes in nonlinear absorbers. Our numerical method compares well with published results. In addition to customary calculation of the transmission curve, we demonstrate the importance of the ESA following the TPA, which may cause significant temporal and radial distortion. We also show that improvements in the transmission can result in significant radial and temporal pulse distortion, which may actually reduce the material effect.