Perovskitas híbridas de haleto sob condições extremas de pressão e temperatura
| Ano de defesa: | 2023 |
|---|---|
| Autor(a) principal: | |
| Orientador(a): | |
| Banca de defesa: | |
| Tipo de documento: | Tese |
| Tipo de acesso: | Acesso aberto |
| Idioma: | por |
| Instituição de defesa: |
Não Informado pela instituição
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| Programa de Pós-Graduação: |
Não Informado pela instituição
|
| Departamento: |
Não Informado pela instituição
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| País: |
Não Informado pela instituição
|
| Palavras-chave em Português: | |
| Link de acesso: | http://www.repositorio.ufc.br/handle/riufc/72478 |
Resumo: | Recently, perovskite-like organic-inorganic hybrid compounds have become promising in developing semiconductors with applications in optoelectronics. Such materials exhibit wide structural versatility and tunable optical properties, either through their intrinsic structural properties or induced by extreme pressure and temperature conditions. In this thesis, we used the slow evaporation method to obtain two new perovskite-like compounds, AlaPbBr3.H2O (Ala= [NH3-CH(NH2)-COOH]+) and (PEA)2Cs2Pb3Br10 (PEA=[C6H5-CH2-CH2-NH3]+), whose structural, optical, and vibrational properties were investigated under extreme conditions of pressure and temperature. In the case of the compound AlaPbBr3.H2O, we observed that its unusual structure [PbBr6]4-, is responsible for forming a wide direct bandgap of Eg = 3.6 eV. Furthermore, substantial evidence supports the hypothesis of self-trapped excitons (STEs) formation. This phenomenon was proven by observing a strong exciton-phonon coupling at low temperatures. In addition, Raman spectroscopy and photoluminescence measurements under high pressures indicated a structural phase transition around 2.2 GPa as the factor responsible for a shift in the emission band energy. In the case of the compound (PEA)2Cs2Pb3Br10, we observed a structure belonging to the Ruddlesden-Popper phase, presenting a direct bandgap of Eg=2.5 eV and an emission profile susceptible to temperature and pressure variations. It is observed that the structural transition around 100K is the mechanism for a sudden change observed in the emission spectrum as a function of temperature. Associated with this phenomenon, the emergence of additional emission peaks around 60K suggests the formation of new electronic recombinations. An attenuated exciton-phonon coupling is also observed, possibly related to the effects of the inorganic layer in its structure. Under pressure, it is observed for this compound that two phase transitions at 0.5 GPa and 2.5 GPa are responsible for the formation and suppression of the emission bands, respectively. Additionally, variations in the number of Raman modes suggest a correlation between pressure-induced distortions in the [PbBr6]4- octahedra and the emission dynamics of this compound. |
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Vasconcelos, Francisco Nailson Farias dePaschoal, Carlos William de Araújo2023-05-24T19:55:13Z2023-05-24T19:55:13Z2023VASCONCELOS, F. N. F. Perovskitas híbridas de haleto sob condições extremas de pressão e temperatura. 2023. 110 f. Tese (Doutorado em Física) - Centro de Ciências, Universidade Federal do Ceará, Fortaleza, 2023.http://www.repositorio.ufc.br/handle/riufc/72478Recently, perovskite-like organic-inorganic hybrid compounds have become promising in developing semiconductors with applications in optoelectronics. Such materials exhibit wide structural versatility and tunable optical properties, either through their intrinsic structural properties or induced by extreme pressure and temperature conditions. In this thesis, we used the slow evaporation method to obtain two new perovskite-like compounds, AlaPbBr3.H2O (Ala= [NH3-CH(NH2)-COOH]+) and (PEA)2Cs2Pb3Br10 (PEA=[C6H5-CH2-CH2-NH3]+), whose structural, optical, and vibrational properties were investigated under extreme conditions of pressure and temperature. In the case of the compound AlaPbBr3.H2O, we observed that its unusual structure [PbBr6]4-, is responsible for forming a wide direct bandgap of Eg = 3.6 eV. Furthermore, substantial evidence supports the hypothesis of self-trapped excitons (STEs) formation. This phenomenon was proven by observing a strong exciton-phonon coupling at low temperatures. In addition, Raman spectroscopy and photoluminescence measurements under high pressures indicated a structural phase transition around 2.2 GPa as the factor responsible for a shift in the emission band energy. In the case of the compound (PEA)2Cs2Pb3Br10, we observed a structure belonging to the Ruddlesden-Popper phase, presenting a direct bandgap of Eg=2.5 eV and an emission profile susceptible to temperature and pressure variations. It is observed that the structural transition around 100K is the mechanism for a sudden change observed in the emission spectrum as a function of temperature. Associated with this phenomenon, the emergence of additional emission peaks around 60K suggests the formation of new electronic recombinations. An attenuated exciton-phonon coupling is also observed, possibly related to the effects of the inorganic layer in its structure. Under pressure, it is observed for this compound that two phase transitions at 0.5 GPa and 2.5 GPa are responsible for the formation and suppression of the emission bands, respectively. Additionally, variations in the number of Raman modes suggest a correlation between pressure-induced distortions in the [PbBr6]4- octahedra and the emission dynamics of this compound.Recentemente, compostos híbridos orgânicos-inorgânicos do tipo perovskita se tornaram promissores no desenvolvimento de semicondutores com aplicações em optoeletrônica. Tais materiais exibem ampla versatilidade estrutural e propriedades ópticas sensivelmente reguláveis, seja por meio de suas propriedades estruturais intrínsecas, ou induzidas por condições extremas de pressão e temperatura. Nesta tese, utilizamos o método de evaporação lenta para a obtenção dois novos compostos híbridos do tipo perovskita, AlaPbBr3.H2O (Ala= [NH3-CH(NH2)-COOH]+) e (PEA)2Cs2Pb3Br10 (PEA=[C6H5-CH2-CH2-NH3]+), cujas propriedades estruturais, ópticas e vibracionais foram investigadas sob condições extremas de pressão e temperatura. No caso do composto AlaPbBr3.H2O, observamos que sua organização incomum de octaedros [PbBr6]4- é responsável pela formação de um bandgap direto de eV. Além disso, fortes evidências corroboraram a hipótese da formação de self-trapped excitons (STE). Tal fenômeno foi comprovado através da observação de um forte acoplamento éxciton-fônon em baixas temperaturas. Além disso, medidas de espectroscopia Raman e de fotoluminescência sob altas pressões apontaram uma transição de fase estrutural em torno de 2,2 GPa como fator responsável pela mudança na energia da banda de emissão. No caso do composto (PEA)2Cs2Pb3Br10, observamos uma estrutura pertencente à fase Ruddlesden-Popper, apresentando um bandgap direto de eV e um perfil de emissão bastante sensível à variações de temperatura e pressão. Observa-se que uma possível transição estrutural em torno de 100 K é o mecanismo para uma mudança abrupta observada no espectro de emissão em função da temperatura. Associado a esse fenômeno, o surgimento de picos de emissão adicionais em torno de 60 K sugerem a formação de novas recombinações eletrônicas. Observa-se também um atenuado acoplamento éxciton-fônon, possivelmente relacionado a efeitos da camada inorgânica em sua estrutura. Já no estudo com pressão, observa-se para esse composto, que duas transições de fase em 0,5 GPa e 2,5 GPa são responsáveis pela formação e supressão, respectivamente, das bandas de emissão. Além disso, variações no número de modos Raman sugerem uma correlação entre distorções induzidas por pressão nos octaedros [PbBr6]4- e a dinâmica de emissão deste composto.PerovskitaEspectroscopia RamanEspectroscopia de fotoluminescênciaPerovskitas híbridas de haleto sob condições extremas de pressão e temperaturainfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/doctoralThesisporreponame:Repositório Institucional da Universidade Federal do Ceará (UFC)instname:Universidade Federal do Ceará (UFC)instacron:UFCinfo:eu-repo/semantics/openAccessORIGINAL2023_tese_fnfvasconcelos.pdf2023_tese_fnfvasconcelos.pdfapplication/pdf8851372http://repositorio.ufc.br/bitstream/riufc/72478/5/2023_tese_fnfvasconcelos.pdfda171cad800783f877991c801f447b35MD55LICENSElicense.txtlicense.txttext/plain; charset=utf-81748http://repositorio.ufc.br/bitstream/riufc/72478/4/license.txt8a4605be74aa9ea9d79846c1fba20a33MD54riufc/724782023-05-24 16:55:56.51oai:repositorio.ufc.br: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Repositório InstitucionalPUBhttp://www.repositorio.ufc.br/ri-oai/requestbu@ufc.br || repositorio@ufc.bropendoar:2023-05-24T19:55:56Repositório Institucional da Universidade Federal do Ceará (UFC) - Universidade Federal do Ceará (UFC)false |
| dc.title.pt_BR.fl_str_mv |
Perovskitas híbridas de haleto sob condições extremas de pressão e temperatura |
| title |
Perovskitas híbridas de haleto sob condições extremas de pressão e temperatura |
| spellingShingle |
Perovskitas híbridas de haleto sob condições extremas de pressão e temperatura Vasconcelos, Francisco Nailson Farias de Perovskita Espectroscopia Raman Espectroscopia de fotoluminescência |
| title_short |
Perovskitas híbridas de haleto sob condições extremas de pressão e temperatura |
| title_full |
Perovskitas híbridas de haleto sob condições extremas de pressão e temperatura |
| title_fullStr |
Perovskitas híbridas de haleto sob condições extremas de pressão e temperatura |
| title_full_unstemmed |
Perovskitas híbridas de haleto sob condições extremas de pressão e temperatura |
| title_sort |
Perovskitas híbridas de haleto sob condições extremas de pressão e temperatura |
| author |
Vasconcelos, Francisco Nailson Farias de |
| author_facet |
Vasconcelos, Francisco Nailson Farias de |
| author_role |
author |
| dc.contributor.author.fl_str_mv |
Vasconcelos, Francisco Nailson Farias de |
| dc.contributor.advisor1.fl_str_mv |
Paschoal, Carlos William de Araújo |
| contributor_str_mv |
Paschoal, Carlos William de Araújo |
| dc.subject.por.fl_str_mv |
Perovskita Espectroscopia Raman Espectroscopia de fotoluminescência |
| topic |
Perovskita Espectroscopia Raman Espectroscopia de fotoluminescência |
| description |
Recently, perovskite-like organic-inorganic hybrid compounds have become promising in developing semiconductors with applications in optoelectronics. Such materials exhibit wide structural versatility and tunable optical properties, either through their intrinsic structural properties or induced by extreme pressure and temperature conditions. In this thesis, we used the slow evaporation method to obtain two new perovskite-like compounds, AlaPbBr3.H2O (Ala= [NH3-CH(NH2)-COOH]+) and (PEA)2Cs2Pb3Br10 (PEA=[C6H5-CH2-CH2-NH3]+), whose structural, optical, and vibrational properties were investigated under extreme conditions of pressure and temperature. In the case of the compound AlaPbBr3.H2O, we observed that its unusual structure [PbBr6]4-, is responsible for forming a wide direct bandgap of Eg = 3.6 eV. Furthermore, substantial evidence supports the hypothesis of self-trapped excitons (STEs) formation. This phenomenon was proven by observing a strong exciton-phonon coupling at low temperatures. In addition, Raman spectroscopy and photoluminescence measurements under high pressures indicated a structural phase transition around 2.2 GPa as the factor responsible for a shift in the emission band energy. In the case of the compound (PEA)2Cs2Pb3Br10, we observed a structure belonging to the Ruddlesden-Popper phase, presenting a direct bandgap of Eg=2.5 eV and an emission profile susceptible to temperature and pressure variations. It is observed that the structural transition around 100K is the mechanism for a sudden change observed in the emission spectrum as a function of temperature. Associated with this phenomenon, the emergence of additional emission peaks around 60K suggests the formation of new electronic recombinations. An attenuated exciton-phonon coupling is also observed, possibly related to the effects of the inorganic layer in its structure. Under pressure, it is observed for this compound that two phase transitions at 0.5 GPa and 2.5 GPa are responsible for the formation and suppression of the emission bands, respectively. Additionally, variations in the number of Raman modes suggest a correlation between pressure-induced distortions in the [PbBr6]4- octahedra and the emission dynamics of this compound. |
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2023 |
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2023-05-24T19:55:13Z |
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2023-05-24T19:55:13Z |
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2023 |
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info:eu-repo/semantics/doctoralThesis |
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VASCONCELOS, F. N. F. Perovskitas híbridas de haleto sob condições extremas de pressão e temperatura. 2023. 110 f. Tese (Doutorado em Física) - Centro de Ciências, Universidade Federal do Ceará, Fortaleza, 2023. |
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http://www.repositorio.ufc.br/handle/riufc/72478 |
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VASCONCELOS, F. N. F. Perovskitas híbridas de haleto sob condições extremas de pressão e temperatura. 2023. 110 f. Tese (Doutorado em Física) - Centro de Ciências, Universidade Federal do Ceará, Fortaleza, 2023. |
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