Estudo de propriedades ópticas não lineares de derivados de dibenzalacetona
Autor(a) principal: | |
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Data de Publicação: | 2019 |
Tipo de documento: | Tese |
Idioma: | por |
Título da fonte: | Repositório Institucional da UFS |
Texto Completo: | http://ri.ufs.br/jspui/handle/riufs/12673 |
Resumo: | Materials with high nonlinear optical properties are of great interest for the field of photonics due to the potentiality of use in several applications, such as 3D micro-fabrication, optical limiting, electro-optical devices, biological probes, photodynamic therapy, etc. In the last years, organic materials with nonlinear optical responses have emerged as promising candidates for diverse photonic applications. One of the main reasons for this potential is relatively easy tailoring of the molecular structure of organic compounds, while compared with inorganic ones, due to the evolution of molecular engineering. These molecular changes induce different linear and nonlinear optical responses, which must be carefully studied to define in which type of photonic device these organic compounds could be applied. In this thesis, a careful study of the change of linear and nonlinear optical responses was carried out as a function of the molecular structure of five organic compounds derived from dibenzalacetone. The nonlinear optical responses investigated corresponding to the second- and third-order processes, namely the first molecular hyperpolarizability (βHRS) and the two-photon absorption cross-section (σA2F ), respectively. The experimental values of βHRS and σA2F were obtained by using hyper-Rayleigh scattering and Z-scan techniques, respectively. The obtained values of βHRS ranging from 24×10−30 cm4statvolt−1 to 42×10−30 cm4statvolt−1. The σA2F spectra were determined by using the Z-scan technique, and the maximum values obtained are between 17 GM and 40 GM. Also, the σA2F spectra were adjusted by the sum over the essential states approach, in which it was possible to extract some important spectroscopic parameters such as the magnitude of the transition dipole moments between the excited states. To increase the interpretation of the presented study, a theoretical study was carried out to the simulated the absorption spectra of one- and two-photons, as well as the first molecular hyperpolarizability. These results were obtained through quantum chemical calculations using the time-dependent density functional theory by using the Gaussian 09 program package. Moreover, two additional programs were used to post-process the values provided by the Gaussian 09 to achieve the final results of the theoretical optical responses. These results allowed to correlate the linear and nonlinear theoretical optical responses of the molecular structures with the experimental ones. The theoretical values obtained for the first molecular hyperpolarizability, spectral behavior of the simulated absorption spectra of oneand two-photons showed good agreement with the experimental ones, indicating that the calculated transitions were similar to those observed experimentally. |
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Santos, Francisco de AssisRodrigues Júnior, José Joatan2020-02-05T20:31:53Z2020-02-05T20:31:53Z2019-07-29SANTOS, Francisco de Assis. Estudo de propriedades ópticas não lineares de derivados de dibenzalacetona. 2019. 107 f. Tese (Doutorado em Física) - Universidade Federal de Sergipe, São Cristóvão, SE, 2019.http://ri.ufs.br/jspui/handle/riufs/12673Materials with high nonlinear optical properties are of great interest for the field of photonics due to the potentiality of use in several applications, such as 3D micro-fabrication, optical limiting, electro-optical devices, biological probes, photodynamic therapy, etc. In the last years, organic materials with nonlinear optical responses have emerged as promising candidates for diverse photonic applications. One of the main reasons for this potential is relatively easy tailoring of the molecular structure of organic compounds, while compared with inorganic ones, due to the evolution of molecular engineering. These molecular changes induce different linear and nonlinear optical responses, which must be carefully studied to define in which type of photonic device these organic compounds could be applied. In this thesis, a careful study of the change of linear and nonlinear optical responses was carried out as a function of the molecular structure of five organic compounds derived from dibenzalacetone. The nonlinear optical responses investigated corresponding to the second- and third-order processes, namely the first molecular hyperpolarizability (βHRS) and the two-photon absorption cross-section (σA2F ), respectively. The experimental values of βHRS and σA2F were obtained by using hyper-Rayleigh scattering and Z-scan techniques, respectively. The obtained values of βHRS ranging from 24×10−30 cm4statvolt−1 to 42×10−30 cm4statvolt−1. The σA2F spectra were determined by using the Z-scan technique, and the maximum values obtained are between 17 GM and 40 GM. Also, the σA2F spectra were adjusted by the sum over the essential states approach, in which it was possible to extract some important spectroscopic parameters such as the magnitude of the transition dipole moments between the excited states. To increase the interpretation of the presented study, a theoretical study was carried out to the simulated the absorption spectra of one- and two-photons, as well as the first molecular hyperpolarizability. These results were obtained through quantum chemical calculations using the time-dependent density functional theory by using the Gaussian 09 program package. Moreover, two additional programs were used to post-process the values provided by the Gaussian 09 to achieve the final results of the theoretical optical responses. These results allowed to correlate the linear and nonlinear theoretical optical responses of the molecular structures with the experimental ones. The theoretical values obtained for the first molecular hyperpolarizability, spectral behavior of the simulated absorption spectra of oneand two-photons showed good agreement with the experimental ones, indicating that the calculated transitions were similar to those observed experimentally.Materiais que apresentam propriedades ópticas não lineares elevadas são de grande interesse para o campo da fotônica devido à potencialidade de utilização em várias aplicações, tais como: microfabricação tridimensional, limitação óptica, dispositivos eletro-ópticos, marcadores biológicos, terapia fotodinâmica, entre outras. Neste contexto, nas últimas décadas, materiais orgânicos com respostas ópticas não lineares, emergiram como candidatos promissores para diversas aplicações fotônicas. Umas das principais razões desse potencial, é a relativa facilidade da alteração da estrutura molecular dos compostos orgânicos, quando comparada a compostos inorgânicos, devido à evolução da engenharia molecular. Essas alterações moleculares induzem diferentes repostas ópticas lineares e não lineares, que deverão ser estudadas cuidadosamente para definir em que tipo de dispositivo fotônico os compostos orgânicos em estudo deverão ser aplicados. Nesta tese, foi realizado um estudo cuidadoso da variação das respostas ópticas lineares e não lineares em função da estrutura molecular de cinco compostos orgânicos derivados da dibenzalacetona. As respostas ópticas não lineares investigadas, corresponderam aos processos de segunda e terceira ordem, mais precisamente a primeira hiperpolarizabilidade molecular (βHRS) e a seção de choque da absorção de dois fótons (σA2F ), respectivamente. Os valores experimentais de βHRS e σA2F foram obtidos através das técnicas de espalhamento de hiper-Rayleigh e de varredura-Z, respectivamente. Os valores de βHRS obtidos variaram de 24×10−30 cm4statvolt−1 a 42×10−30 cm4statvolt−1. Através da técnica de varredura-Z, foram determinados os espectros de σA2F , os quais apresentaram amplitudes máxima entre 17 GM a 40 GM. Além disso, os espectros de σA2F foram ajustados através do método da soma sobre os estados essenciais, no qual foi possível extrair importantes parâmetros espectroscópicos, tais como: a magnitude dos momentos de dipolo de transição entre os estados excitados. De forma a incrementar o detalhamento do estudo apresentado, foram obtidos resultados teóricos tais como os espectros simulados de absorção de um e dois fótons, e os valores teóricos da primeira hiperpolarizabilidade molecular. Tais resultados foram obtidos através de cálculos químico-quânticos empregando a teoria do funcional de densidade dependente do tempo, usando o programa Gaussian 09, com o auxílio da utilização de dois programas de pós-processamento dos valores fornecidos pelo Gaussian 09. Estes resultados teóricos permitiram correlacionar as respostas ópticas lineares e não lineares das estruturas moleculares, com os resultados experimentais. Os valores teóricos obtidos para primeira hiperpolarizabilidade revelaram-se dentro do limite da margem de erro dos resultados experimentais. Enquanto que, a forma de linha dos espectros simulados da absorção de um e dois fótons apresentaram boa concordância com os espectros experimentais, indicando que as transições calculadas foram semelhantes as observadas experimentalmente.Coordenação de Aperfeiçoamento de Pessoal de Nível Superior - CAPESSão Cristóvão, SEporÓptica não linearMoléculas orgânicasDibenzalacetonasAbsorção de dois fótonsEspalhamento hiper-RayleighDerivados de dibenzalacetonasPrimeira hiperpolarizabilidade molecularVarredura-ZOrganic moleculesDibenzylideneacetone derivativesFirst molecular hyperpolarizabilityTwo-photon absorptionHyper-Rayleigh scatteringZ-scanCIENCIAS EXATAS E DA TERRA::FISICAEstudo de propriedades ópticas não lineares de derivados de dibenzalacetonainfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/doctoralThesisPós-Graduação em FísicaUniversidade Federal de Sergipereponame:Repositório Institucional da UFSinstname:Universidade Federal de Sergipe (UFS)instacron:UFSinfo:eu-repo/semantics/openAccessTEXTFRANCISCO_ASSIS_SANTOS.pdf.txtFRANCISCO_ASSIS_SANTOS.pdf.txtExtracted texttext/plain163135https://ri.ufs.br/jspui/bitstream/riufs/12673/3/FRANCISCO_ASSIS_SANTOS.pdf.txt09f9b70e08f7738effab9cc910aae4cfMD53THUMBNAILFRANCISCO_ASSIS_SANTOS.pdf.jpgFRANCISCO_ASSIS_SANTOS.pdf.jpgGenerated Thumbnailimage/jpeg1676https://ri.ufs.br/jspui/bitstream/riufs/12673/4/FRANCISCO_ASSIS_SANTOS.pdf.jpg1efdbff2c72e166b0ef2ace4d3d4e108MD54ORIGINALFRANCISCO_ASSIS_SANTOS.pdfFRANCISCO_ASSIS_SANTOS.pdfapplication/pdf37849135https://ri.ufs.br/jspui/bitstream/riufs/12673/2/FRANCISCO_ASSIS_SANTOS.pdfa69a7d4423b9c7ca3217e53bc4275206MD52LICENSElicense.txtlicense.txttext/plain; charset=utf-81475https://ri.ufs.br/jspui/bitstream/riufs/12673/1/license.txt098cbbf65c2c15e1fb2e49c5d306a44cMD51riufs/126732020-02-05 17:31:53.5oai:ufs.br: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Repositório InstitucionalPUBhttps://ri.ufs.br/oai/requestrepositorio@academico.ufs.bropendoar:2020-02-05T20:31:53Repositório Institucional da UFS - Universidade Federal de Sergipe (UFS)false |
dc.title.pt_BR.fl_str_mv |
Estudo de propriedades ópticas não lineares de derivados de dibenzalacetona |
title |
Estudo de propriedades ópticas não lineares de derivados de dibenzalacetona |
spellingShingle |
Estudo de propriedades ópticas não lineares de derivados de dibenzalacetona Santos, Francisco de Assis Óptica não linear Moléculas orgânicas Dibenzalacetonas Absorção de dois fótons Espalhamento hiper-Rayleigh Derivados de dibenzalacetonas Primeira hiperpolarizabilidade molecular Varredura-Z Organic molecules Dibenzylideneacetone derivatives First molecular hyperpolarizability Two-photon absorption Hyper-Rayleigh scattering Z-scan CIENCIAS EXATAS E DA TERRA::FISICA |
title_short |
Estudo de propriedades ópticas não lineares de derivados de dibenzalacetona |
title_full |
Estudo de propriedades ópticas não lineares de derivados de dibenzalacetona |
title_fullStr |
Estudo de propriedades ópticas não lineares de derivados de dibenzalacetona |
title_full_unstemmed |
Estudo de propriedades ópticas não lineares de derivados de dibenzalacetona |
title_sort |
Estudo de propriedades ópticas não lineares de derivados de dibenzalacetona |
author |
Santos, Francisco de Assis |
author_facet |
Santos, Francisco de Assis |
author_role |
author |
dc.contributor.author.fl_str_mv |
Santos, Francisco de Assis |
dc.contributor.advisor1.fl_str_mv |
Rodrigues Júnior, José Joatan |
contributor_str_mv |
Rodrigues Júnior, José Joatan |
dc.subject.por.fl_str_mv |
Óptica não linear Moléculas orgânicas Dibenzalacetonas Absorção de dois fótons Espalhamento hiper-Rayleigh Derivados de dibenzalacetonas Primeira hiperpolarizabilidade molecular Varredura-Z |
topic |
Óptica não linear Moléculas orgânicas Dibenzalacetonas Absorção de dois fótons Espalhamento hiper-Rayleigh Derivados de dibenzalacetonas Primeira hiperpolarizabilidade molecular Varredura-Z Organic molecules Dibenzylideneacetone derivatives First molecular hyperpolarizability Two-photon absorption Hyper-Rayleigh scattering Z-scan CIENCIAS EXATAS E DA TERRA::FISICA |
dc.subject.eng.fl_str_mv |
Organic molecules Dibenzylideneacetone derivatives First molecular hyperpolarizability Two-photon absorption Hyper-Rayleigh scattering Z-scan |
dc.subject.cnpq.fl_str_mv |
CIENCIAS EXATAS E DA TERRA::FISICA |
description |
Materials with high nonlinear optical properties are of great interest for the field of photonics due to the potentiality of use in several applications, such as 3D micro-fabrication, optical limiting, electro-optical devices, biological probes, photodynamic therapy, etc. In the last years, organic materials with nonlinear optical responses have emerged as promising candidates for diverse photonic applications. One of the main reasons for this potential is relatively easy tailoring of the molecular structure of organic compounds, while compared with inorganic ones, due to the evolution of molecular engineering. These molecular changes induce different linear and nonlinear optical responses, which must be carefully studied to define in which type of photonic device these organic compounds could be applied. In this thesis, a careful study of the change of linear and nonlinear optical responses was carried out as a function of the molecular structure of five organic compounds derived from dibenzalacetone. The nonlinear optical responses investigated corresponding to the second- and third-order processes, namely the first molecular hyperpolarizability (βHRS) and the two-photon absorption cross-section (σA2F ), respectively. The experimental values of βHRS and σA2F were obtained by using hyper-Rayleigh scattering and Z-scan techniques, respectively. The obtained values of βHRS ranging from 24×10−30 cm4statvolt−1 to 42×10−30 cm4statvolt−1. The σA2F spectra were determined by using the Z-scan technique, and the maximum values obtained are between 17 GM and 40 GM. Also, the σA2F spectra were adjusted by the sum over the essential states approach, in which it was possible to extract some important spectroscopic parameters such as the magnitude of the transition dipole moments between the excited states. To increase the interpretation of the presented study, a theoretical study was carried out to the simulated the absorption spectra of one- and two-photons, as well as the first molecular hyperpolarizability. These results were obtained through quantum chemical calculations using the time-dependent density functional theory by using the Gaussian 09 program package. Moreover, two additional programs were used to post-process the values provided by the Gaussian 09 to achieve the final results of the theoretical optical responses. These results allowed to correlate the linear and nonlinear theoretical optical responses of the molecular structures with the experimental ones. The theoretical values obtained for the first molecular hyperpolarizability, spectral behavior of the simulated absorption spectra of oneand two-photons showed good agreement with the experimental ones, indicating that the calculated transitions were similar to those observed experimentally. |
publishDate |
2019 |
dc.date.issued.fl_str_mv |
2019-07-29 |
dc.date.accessioned.fl_str_mv |
2020-02-05T20:31:53Z |
dc.date.available.fl_str_mv |
2020-02-05T20:31:53Z |
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info:eu-repo/semantics/publishedVersion |
dc.type.driver.fl_str_mv |
info:eu-repo/semantics/doctoralThesis |
format |
doctoralThesis |
status_str |
publishedVersion |
dc.identifier.citation.fl_str_mv |
SANTOS, Francisco de Assis. Estudo de propriedades ópticas não lineares de derivados de dibenzalacetona. 2019. 107 f. Tese (Doutorado em Física) - Universidade Federal de Sergipe, São Cristóvão, SE, 2019. |
dc.identifier.uri.fl_str_mv |
http://ri.ufs.br/jspui/handle/riufs/12673 |
identifier_str_mv |
SANTOS, Francisco de Assis. Estudo de propriedades ópticas não lineares de derivados de dibenzalacetona. 2019. 107 f. Tese (Doutorado em Física) - Universidade Federal de Sergipe, São Cristóvão, SE, 2019. |
url |
http://ri.ufs.br/jspui/handle/riufs/12673 |
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Pós-Graduação em Física |
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Universidade Federal de Sergipe |
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