Studying the first order hyperpolarizability spectra in chalcone-based derivatives and the relation with one- and two-photon absorption transitions.

The first-order molecular hyperpolarizability (ß) dispersion was measured in seven chalcone-based molecules utilizing the tunable femtosecond hyper-Rayleigh scattering (tHRS) technique. Additionally, a theoretical model based on photophysical parameters was employed to better understand ß dispersion. Due to the distinct substitution patterns of the aryl/heteroaryl rings within the chalcone structure, varying profiles of one- and two-photon absorption spectra and ß dispersion were observed. The applied model highlighted two important factors contributing to achieving high ß values: (i) the presence of red-shifted one-photon and two-photon absorption bands; and (ii) the number of discernible absorption bands. To contextualize these results with other molecular structures, we employed the HRS figure of merit (FOM). Remarkably, it was revealed that chemically engineered small chalcone molecules exhibit a FOM comparable to larger quadrupolar and octupolar ones. This underscores the significance of tHRS scattering measurements and their correlation with absorptive parameters in the design and characterization of nonlinear optical materials.

Enhancement of optical properties of new purine nucleobases containing electron-donating and -withdrawing peripheral groups.

Nowadays, a great deal of attention has been focused on synthesizing highly fluorescent unnatural base analogs. This has been motivated by the need to overcome the lack of fluorescence of nucleic acids' natural bases. Fluorescent unnatural base analogs, such as purines, may be used in several applications, such as DNA or RNA optical spectroscopy studies. Moreover, for purines base analogs, the optical properties, for example, emission, can be tunable through molecular engineering, improving their applications as fluorescent probes. Looking in this direction, the synthesis and optical spectroscopic studies of a new set of purines base analogs are of foremost relevance. Here, an increase in the fluorescence quantum yield was observed in molecules with NH-π-CN arrangement. The two-photon absorption (2PA) cross-sections also increased for the lower energy 2PA state. The enhancement of both properties results in a two-photon brightness of 5 and 10 times higher than in compounds lacking the NH-π-CN arrangement. For the higher energy 2PA state, an excited state absorption contribution to the 2PA cross-section values was observed, that was verified through ultrafast transient absorption measurements. The higher 2PA brightness makes the purines base analogs promising candidates as fluorescent probes in RNA and DNA spectroscopic studies.