Observation of the two-photon transition enhanced first hyperpolarizability spectra in cinnamaldehyde derivatives: A femtosecond regime study.

The application of nonlinear optical effects in optoelectronic devices is still scarce because the irradiance threshold necessary to induce a specific effect is very high. In this context, knowing the frequency-resolved first order molecular hyperpolarizability (β) is essential to identifying regions where this response is intense enough to allow for applications in commercial devices. Thus, herein, we have determined the β spectral dependence of five new push-pull cinnamylidene acetophenone derivatives using femtosecond laser-induced Hyper-Rayleigh Scattering (HRS). A considerable increase in β values was observed in molecules. We found remarkable β values in regions near the two-photon resonance, which are mediated by electron withdrawing and donating groups. This effect was mapped using wavelength-tunable femtosecond Z-scan technique. Furthermore, it was modeled in light of the sum-over-states approach for the second- and third-order nonlinearities. Finally, our outcomes suggest a strategy to obtain large β values mediated by the 2PA transition.