Spectral dependence of nonlinear optical properties of symmetrical octatetraynes with p-substituted phenyl end-groups.

Organic compounds containing conjugated carbon chains have been extensively investigated due to their interesting properties including nonlinear optical response. Polyynes are a group of compounds where the conjugation can be modified by appropriate selection of end-groups, enabling "control" and improvement of nonlinear effects. In this work, we investigate three newly synthesized aryl end-capped octatetraynes, exhibiting strong nonlinear absorption and nonlinear refraction properties, which can be attributed to the presence of aryl end-groups with electron-withdrawing functional groups suitable for further extending the conjugation. Nonlinear optical measurements were performed using a f-scan (modified Z-scan) technique with a femtosecond laser system at various wavelengths in the visible and near-infrared range (540-1600 nm), revealing strong negative third-order nonlinear refraction (3NR) and two-photon absorption (2PA) below 600 nm and a noticeable three-photon absorption (3PA) at longer wavelengths. The results of spectroscopic characterization and the crystallographic data for the investigated compounds are also presented.