Fine Structure Splitting of Phonon-Assisted Excitonic Transition in (PEA)2PbI4 Two-Dimensional Perovskites
Two-dimensional van der Waals materials exhibit particularly strong excitonic effects, which causes them to be an exceptionally interesting platform for the investigation of exciton physics. A notable example is the two-dimensional Ruddlesden–Popper perovskites, where quantum and dielectri...
| Main Authors: | , , , , , , , , , |
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| Format: | Article |
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Multidisciplinary Digital Publishing Institute
2023
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| Online Access: | https://hdl.handle.net/1721.1/148835 |
| _version_ | 1826195986594136064 |
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| author | Posmyk, Katarzyna Dyksik, Mateusz Surrente, Alessandro Zalewska, Katarzyna Śmiertka, Maciej Cybula, Ewelina Paritmongkol, Watcharaphol Tisdale, William A. Plochocka, Paulina Baranowski, Michał |
| author2 | Massachusetts Institute of Technology. Department of Chemical Engineering |
| author_facet | Massachusetts Institute of Technology. Department of Chemical Engineering Posmyk, Katarzyna Dyksik, Mateusz Surrente, Alessandro Zalewska, Katarzyna Śmiertka, Maciej Cybula, Ewelina Paritmongkol, Watcharaphol Tisdale, William A. Plochocka, Paulina Baranowski, Michał |
| author_sort | Posmyk, Katarzyna |
| collection | MIT |
| description | Two-dimensional van der Waals materials exhibit particularly strong excitonic effects, which causes them to be an exceptionally interesting platform for the investigation of exciton physics. A notable example is the two-dimensional Ruddlesden–Popper perovskites, where quantum and dielectric confinement together with soft, polar, and low symmetry lattice create a unique background for electron and hole interaction. Here, with the use of polarization-resolved optical spectroscopy, we have demonstrated that the simultaneous presence of tightly bound excitons, together with strong exciton–phonon coupling, allows for observing the exciton fine structure splitting of the phonon-assisted transitions of two-dimensional perovskite (PEA)<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mn>2</mn></msub></semantics></math></inline-formula>PbI<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mn>4</mn></msub></semantics></math></inline-formula>, where PEA stands for phenylethylammonium. We demonstrate that the phonon-assisted sidebands characteristic for (PEA)<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mn>2</mn></msub></semantics></math></inline-formula>PbI<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mn>4</mn></msub></semantics></math></inline-formula> are split and linearly polarized, mimicking the characteristics of the corresponding zero-phonon lines. Interestingly, the splitting of differently polarized phonon-assisted transitions can be different from that of the zero-phonon lines. We attribute this effect to the selective coupling of linearly polarized exciton states to non-degenerate phonon modes of different symmetries resulting from the low symmetry of (PEA)<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mn>2</mn></msub></semantics></math></inline-formula>PbI<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mn>4</mn></msub></semantics></math></inline-formula> lattice. |
| first_indexed | 2024-09-23T10:19:03Z |
| format | Article |
| id | mit-1721.1/148835 |
| institution | Massachusetts Institute of Technology |
| last_indexed | 2024-09-23T10:19:03Z |
| publishDate | 2023 |
| publisher | Multidisciplinary Digital Publishing Institute |
| record_format | dspace |
| spelling | mit-1721.1/1488352024-01-10T18:04:48Z Fine Structure Splitting of Phonon-Assisted Excitonic Transition in (PEA)2PbI4 Two-Dimensional Perovskites Posmyk, Katarzyna Dyksik, Mateusz Surrente, Alessandro Zalewska, Katarzyna Śmiertka, Maciej Cybula, Ewelina Paritmongkol, Watcharaphol Tisdale, William A. Plochocka, Paulina Baranowski, Michał Massachusetts Institute of Technology. Department of Chemical Engineering Two-dimensional van der Waals materials exhibit particularly strong excitonic effects, which causes them to be an exceptionally interesting platform for the investigation of exciton physics. A notable example is the two-dimensional Ruddlesden–Popper perovskites, where quantum and dielectric confinement together with soft, polar, and low symmetry lattice create a unique background for electron and hole interaction. Here, with the use of polarization-resolved optical spectroscopy, we have demonstrated that the simultaneous presence of tightly bound excitons, together with strong exciton–phonon coupling, allows for observing the exciton fine structure splitting of the phonon-assisted transitions of two-dimensional perovskite (PEA)<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mn>2</mn></msub></semantics></math></inline-formula>PbI<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mn>4</mn></msub></semantics></math></inline-formula>, where PEA stands for phenylethylammonium. We demonstrate that the phonon-assisted sidebands characteristic for (PEA)<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mn>2</mn></msub></semantics></math></inline-formula>PbI<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mn>4</mn></msub></semantics></math></inline-formula> are split and linearly polarized, mimicking the characteristics of the corresponding zero-phonon lines. Interestingly, the splitting of differently polarized phonon-assisted transitions can be different from that of the zero-phonon lines. We attribute this effect to the selective coupling of linearly polarized exciton states to non-degenerate phonon modes of different symmetries resulting from the low symmetry of (PEA)<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mn>2</mn></msub></semantics></math></inline-formula>PbI<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mn>4</mn></msub></semantics></math></inline-formula> lattice. 2023-03-28T20:51:58Z 2023-03-28T20:51:58Z 2023-03-21 2023-03-28T12:55:50Z Article http://purl.org/eprint/type/JournalArticle https://hdl.handle.net/1721.1/148835 Nanomaterials 13 (6): 1119 (2023) PUBLISHER_CC http://dx.doi.org/10.3390/nano13061119 Creative Commons Attribution http://creativecommons.org/licenses/by/4.0/ application/pdf Multidisciplinary Digital Publishing Institute Multidisciplinary Digital Publishing Institute |
| spellingShingle | Posmyk, Katarzyna Dyksik, Mateusz Surrente, Alessandro Zalewska, Katarzyna Śmiertka, Maciej Cybula, Ewelina Paritmongkol, Watcharaphol Tisdale, William A. Plochocka, Paulina Baranowski, Michał Fine Structure Splitting of Phonon-Assisted Excitonic Transition in (PEA)2PbI4 Two-Dimensional Perovskites |
| title | Fine Structure Splitting of Phonon-Assisted Excitonic Transition in (PEA)2PbI4 Two-Dimensional Perovskites |
| title_full | Fine Structure Splitting of Phonon-Assisted Excitonic Transition in (PEA)2PbI4 Two-Dimensional Perovskites |
| title_fullStr | Fine Structure Splitting of Phonon-Assisted Excitonic Transition in (PEA)2PbI4 Two-Dimensional Perovskites |
| title_full_unstemmed | Fine Structure Splitting of Phonon-Assisted Excitonic Transition in (PEA)2PbI4 Two-Dimensional Perovskites |
| title_short | Fine Structure Splitting of Phonon-Assisted Excitonic Transition in (PEA)2PbI4 Two-Dimensional Perovskites |
| title_sort | fine structure splitting of phonon assisted excitonic transition in pea 2pbi4 two dimensional perovskites |
| url | https://hdl.handle.net/1721.1/148835 |
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