Fine Structure Splitting of Phonon-Assisted Excitonic Transition in (PEA)<sub>2</sub>PbI<sub>4</sub> 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 dielectric confinem...
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MDPI AG
2023-03-01
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| Series: | Nanomaterials |
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| Online Access: | https://www.mdpi.com/2079-4991/13/6/1119 |
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| author | Katarzyna Posmyk Mateusz Dyksik Alessandro Surrente Katarzyna Zalewska Maciej Śmiertka Ewelina Cybula Watcharaphol Paritmongkol William A. Tisdale Paulina Plochocka Michał Baranowski |
| author_facet | Katarzyna Posmyk Mateusz Dyksik Alessandro Surrente Katarzyna Zalewska Maciej Śmiertka Ewelina Cybula Watcharaphol Paritmongkol William A. Tisdale Paulina Plochocka Michał Baranowski |
| author_sort | Katarzyna Posmyk |
| collection | DOAJ |
| 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. |
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| series | Nanomaterials |
| spelling | doaj.art-3ad9b0bef7ce43ae99670fb3033d0ead2023-11-17T13:01:48ZengMDPI AGNanomaterials2079-49912023-03-01136111910.3390/nano13061119Fine Structure Splitting of Phonon-Assisted Excitonic Transition in (PEA)<sub>2</sub>PbI<sub>4</sub> Two-Dimensional PerovskitesKatarzyna Posmyk0Mateusz Dyksik1Alessandro Surrente2Katarzyna Zalewska3Maciej Śmiertka4Ewelina Cybula5Watcharaphol Paritmongkol6William A. Tisdale7Paulina Plochocka8Michał Baranowski9Department of Experimental Physics, Faculty of Fundamental Problems of Technology, Wroclaw University of Science and Technology, 50-370 Wroclaw, PolandDepartment of Experimental Physics, Faculty of Fundamental Problems of Technology, Wroclaw University of Science and Technology, 50-370 Wroclaw, PolandDepartment of Experimental Physics, Faculty of Fundamental Problems of Technology, Wroclaw University of Science and Technology, 50-370 Wroclaw, PolandDepartment of Experimental Physics, Faculty of Fundamental Problems of Technology, Wroclaw University of Science and Technology, 50-370 Wroclaw, PolandDepartment of Experimental Physics, Faculty of Fundamental Problems of Technology, Wroclaw University of Science and Technology, 50-370 Wroclaw, PolandDepartment of Experimental Physics, Faculty of Fundamental Problems of Technology, Wroclaw University of Science and Technology, 50-370 Wroclaw, PolandDepartment of Chemical Engineering, Massachusetts Institute of Technology, Cambridge, MA 02139, USADepartment of Chemical Engineering, Massachusetts Institute of Technology, Cambridge, MA 02139, USADepartment of Experimental Physics, Faculty of Fundamental Problems of Technology, Wroclaw University of Science and Technology, 50-370 Wroclaw, PolandDepartment of Experimental Physics, Faculty of Fundamental Problems of Technology, Wroclaw University of Science and Technology, 50-370 Wroclaw, PolandTwo-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.https://www.mdpi.com/2079-4991/13/6/11192D perovskitesexcitonphononoptical spectroscopyfine structure splitting(PEA)2PbI4 |
| spellingShingle | Katarzyna Posmyk Mateusz Dyksik Alessandro Surrente Katarzyna Zalewska Maciej Śmiertka Ewelina Cybula Watcharaphol Paritmongkol William A. Tisdale Paulina Plochocka Michał Baranowski Fine Structure Splitting of Phonon-Assisted Excitonic Transition in (PEA)<sub>2</sub>PbI<sub>4</sub> Two-Dimensional Perovskites Nanomaterials 2D perovskites exciton phonon optical spectroscopy fine structure splitting (PEA)2PbI4 |
| title | Fine Structure Splitting of Phonon-Assisted Excitonic Transition in (PEA)<sub>2</sub>PbI<sub>4</sub> Two-Dimensional Perovskites |
| title_full | Fine Structure Splitting of Phonon-Assisted Excitonic Transition in (PEA)<sub>2</sub>PbI<sub>4</sub> Two-Dimensional Perovskites |
| title_fullStr | Fine Structure Splitting of Phonon-Assisted Excitonic Transition in (PEA)<sub>2</sub>PbI<sub>4</sub> Two-Dimensional Perovskites |
| title_full_unstemmed | Fine Structure Splitting of Phonon-Assisted Excitonic Transition in (PEA)<sub>2</sub>PbI<sub>4</sub> Two-Dimensional Perovskites |
| title_short | Fine Structure Splitting of Phonon-Assisted Excitonic Transition in (PEA)<sub>2</sub>PbI<sub>4</sub> Two-Dimensional Perovskites |
| title_sort | fine structure splitting of phonon assisted excitonic transition in pea sub 2 sub pbi sub 4 sub two dimensional perovskites |
| topic | 2D perovskites exciton phonon optical spectroscopy fine structure splitting (PEA)2PbI4 |
| url | https://www.mdpi.com/2079-4991/13/6/1119 |
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