Off-resonant third-order optical nonlinearities of squarylium and croconium dyes

The magnitude and dynamic response of the third-order optical nonlinearities of squarylium and croconium dyes in methanol solution were measured by femtosecond degenerate four-wave mixing (DFWM) technique at 800 nm. Ultrafast nonlinear optical responses have been observed, and the magnitude of the second-order hyperpolarizabilities was evaluated to be 5.80 x 10(-31) esu for the squarylium dye and 8.69 x 10(-31) esu for the croconium dye, respectively. The large optical nonlinearities of the dyes can be attributed to their rigid and intramolecular charge transfer structure, and the instantaneous NLO responses of dyes are shorter than the experimental time resolution (50 fs), which is mainly contributed from the electron delocalization. The fast nonlinear response and large third-order optical nonlinearities show that the studied squarylium and croconium dyes might a kind of promising materials for the applications in all-optical switching and modulator.