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

Lucas F Sciuti; Carlos H D Dos Santos; Leandro H Z Cocca; André G Pelosi; Rafaela G M da Costa; Jones Limberger; Cleber R Mendonça; Leonardo De Boni

doi:10.1063/5.0166036

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

J Chem Phys. 2023 Dec 28;159(24):244311. doi: 10.1063/5.0166036.

Authors

Lucas F Sciuti¹, Carlos H D Dos Santos¹, Leandro H Z Cocca¹, André G Pelosi¹, Rafaela G M da Costa², Jones Limberger², Cleber R Mendonça¹, Leonardo De Boni¹

Affiliations

¹ São Carlos Institute of Physics, University of São Paulo, São Carlos, 13560-970 São Paulo, Brazil.
² Departamento de Química, Pontifícia Universidade Católica do Rio de Janeiro, Rua Marquês de São Vicente, 225, 22451-900 Rio de Janeiro, Brazil.

PMID: 38153155
DOI: 10.1063/5.0166036

Abstract

The first-order molecular hyperpolarizability (β) 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 β 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 β dispersion were observed. The applied model highlighted two important factors contributing to achieving high β 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.