Optical limiting and dynamical two-photon absorption of porphyrin with ruthenium outlying complexes for a picosecond pulse train

Propagation and nonlinear optical absorption of a picosecond pulse train in strong reverse saturable absorption (RSA) materials (free-based tetrapyridyl porphyrin H2TPyP with ruthenium (Ru) outlying complexes) are investigated by solving coupled rate equations and field intensity equation. Influence of outlying Ru groups on optical limiting (OL) properties is studied. Propagation of the front subpulses is mainly affected by linear transition between the ground state and the first excited singlet state, while intensity of the latter subpulses is attenuated by the excited state absorption (ESA). These two different absorption mechanisms result in asymmetric distribution of the transmitted pulse. It is shown that effective population transfer time from the ground state to the lowest triplet state and RSA play important roles in the OL performance and pulse shaping. Moreover, our results indicate that the porphyrins studied are ideal optical limiters because of their large ESA cross section and long lifetime of the lowest triplet state. Compounds with the presence of Ru group possess preferable power limiting ability. Ligand group attached to Ru also influences the nonlinear optical absorption of compounds. Special attention has been paid on dynamical two-photon absorption (TPA) cross section which depends crucially on the duration of the subpulse as well as time interval between subpulses. The present study provides a way to modulate nonlinear optical absorption properties of the medium by changing parameters of the pulse train