Elucidating the Photophysics and Nonlinear Optical Properties of a Novel Azo Prototype for Possible Photonic Applications: A Quantum Chemical Analysis
The photophysics and nonlinear optical responses of a novel nitrothiazol-methoxyphenol molecule were investigated using density functional theory (DFT) and time-dependent density functional theory (TD-DFT) methods with the polarizable continuum model to take the solvent effect into account. Special attention is paid to the description of the lowest absorption band, characterized as a strong π → π* state in the visible region of the spectrum. The TD-DFT emission spectrum analysis reveals a significant Stokes shift of more than 120 nm for the π → π* state in gas phase condition. The results show a great influence of the solvent polarity on the nonlinear optical (NLO) response of the molecule. Specifically, the second harmonic generation hyperpolarizability β(-2ω; ω, ω) shows a large variation from gas to aqueous solvent (82 × 10<sup>-30</sup> to 162 × 10<sup>-30</sup> esu), exhibiting notably higher values than those reported for standard compounds such as urea (0.34 × 10<sup>-30</sup> esu) and <i>p</i>-nitroaniline (6.42 × 10<sup>-30</sup> esu). Furthermore, a two-photon absorption analysis indicates a large cross-section (δ<sup>2PA</sup> = 77 GM) with superior performance compared to several dyes. These results make the molecule quite interesting for nonlinear optics.
Authors
- Rodrigo Gester (ORCID: https://orcid.org/0000-0001-6110-424X)
- Herbert C. Georg (ORCID: https://orcid.org/0000-0001-5788-0094)
- Kaline Coutinho (ORCID: https://orcid.org/0000-0002-7586-3324)
- Sylvio Canuto (ORCID: https://orcid.org/0000-0002-9942-8714)
- Neidy S. S. dos Santos (ORCID: https://orcid.org/0000-0002-0177-8004)
- Tertius Lima Fonseca (ORCID: https://orcid.org/0000-0001-5501-7801)
- Patricio F. Provasi (ORCID: https://orcid.org/0000-0002-9773-5542)
- Antônio R. da Cunha (ORCID: https://orcid.org/0000-0002-6280-8772)
- Sávio Fonseca (ORCID: https://orcid.org/0000-0003-1153-8749)
Institutions
- Consejo Nacional de Investigaciones Científicas y Técnicas (AR)
- Universidade de São Paulo (BR)
- National University of the Northeast (AR)
- Universidade Federal do Sul e Sudeste do Pará (BR)
- Universidade Federal do Maranhão (BR)
- Universidade Federal de Goiás (BR)
Publication Details
- Journal
- ACS Omega
- Published
- 2024-09-20
- DOI
- https://doi.org/10.1021/acsomega.4c04240
- Citations
- 4
- Primary Topic
- Nonlinear Optical Materials Studies
- Type
- article
- Field-Weighted Citation Impact
- 0.74
Funders
- Fundação de Amparo à Pesquisa do Estado de São Paulo
- Coordenação de Aperfeiçoamento de Pessoal de Nível Superior
- Consejo Nacional de Investigaciones Científicas y Técnicas
- Fundação de Amparo à Pesquisa do Estado de Alagoas
- Conselho Nacional de Desenvolvimento Científico e Tecnológico
- Fundação de Amparo à Pesquisa e ao Desenvolvimento Científico e Tecnológico do Maranhão
- Fundação Amazônia Paraense de Amparo à Pesquisa
- Universidad Nacional del Nordeste
- Instituto Nacional de Ciência e Tecnologia de Fluidos Complexos