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

Author(s)

Sciuti, Lucas F. ; dos Santos, Carlos H. D. ; Cocca, Leandro H. Z. ; Pelosi, Andre G. ; da Costa, Rafaela G. M. ; Limberger, Jones ; Mendonca, Cleber R. ; De Boni, Leonardo

• Document type: Journal article
• Source: Journal of Chemical Physics; v. 159, n. 24, p. 9-pg., 2023-12-28.

Abstract

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

• FAPESP's process: 11/12399-0 - Femtosecond pulses applied to nonlinear optics: spectroscopy, pulse shaping and microfabrication
• Grantee: Cleber Renato Mendonça
• Support Opportunities: Research Projects - Thematic Grants
• FAPESP's process: 18/11283-7 - Nonlinear photonics: spectroscopy and advanced processing of materials
• Grantee: Cleber Renato Mendonça
• Support Opportunities: Research Projects - Thematic Grants
• FAPESP's process: 16/20886-1 - Ultrafast nonlinear optical spectroscopy: Transient Absorption and optical Kerr Gate with polarization control
• Grantee: Leonardo de Boni
• Support Opportunities: Regular Research Grants
• FAPESP's process: 15/20032-0 - Study on Nonlinear and Charge Transport Properties of Multi-branched Molecules via Quantum Chemical Methods.
• Grantee: Daniel Luiz da Silva
• Support Opportunities: Regular Research Grants