Indirect tail states formation by thermal-induced polar fluctuations in halide perovskites
Halide perovskites possess enormous potential for various optoelectronic applications. Presently, a clear understanding of the interplay between the lattice and electronic effects is still elusive. Specifically, the weakly absorbing tail states and dual emission from perovskites are not satisfactori...
| Main Authors: | , , , , , , , , , , , , , , , |
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| Format: | Journal Article |
| Language: | English |
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2019
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| Online Access: | https://hdl.handle.net/10356/89862 http://hdl.handle.net/10220/47743 |
| _version_ | 1826121932031918080 |
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| author | Wu, Bo Yuan, Haifeng Xu, Qiang Steele, Julian A. Giovanni, David Puech, Pascal Fu, Jianhui Ng, Yan Fong Nur Fadilah Jamaludin Solanki, Ankur Mhaisalkar, Subodh Mathews, Nripan Roeffaers, Maarten B. J. Grätzel, Michael Hofkens, Johan Sum, Tze Chien |
| author2 | School of Materials Science & Engineering |
| author_facet | School of Materials Science & Engineering Wu, Bo Yuan, Haifeng Xu, Qiang Steele, Julian A. Giovanni, David Puech, Pascal Fu, Jianhui Ng, Yan Fong Nur Fadilah Jamaludin Solanki, Ankur Mhaisalkar, Subodh Mathews, Nripan Roeffaers, Maarten B. J. Grätzel, Michael Hofkens, Johan Sum, Tze Chien |
| author_sort | Wu, Bo |
| collection | NTU |
| description | Halide perovskites possess enormous potential for various optoelectronic applications. Presently, a clear understanding of the interplay between the lattice and electronic effects is still elusive. Specifically, the weakly absorbing tail states and dual emission from perovskites are not satisfactorily described by existing theories based on the Urbach tail and reabsorption effect. Herein, through temperature-dependent and time-resolved spectroscopy on metal halide perovskite single crystals with organic or inorganic A-site cations, we confirm the existence of indirect tail states below the direct transition edge to arise from a dynamical Rashba splitting effect, caused by the PbBr6 octahedral thermal polar distortions at elevated temperatures. This dynamic effect is distinct from the static Rashba splitting effect, caused by non-spherical A-site cations or surface induced lattice distortions. Our findings shed fresh perspectives on the electronic-lattice relations paramount for the design and optimization of emergent perovskites, revealing broad implications for light harvesting/photo-detection and light emission/lasing applications. |
| first_indexed | 2024-10-01T05:40:14Z |
| format | Journal Article |
| id | ntu-10356/89862 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T05:40:14Z |
| publishDate | 2019 |
| record_format | dspace |
| spelling | ntu-10356/898622023-02-28T19:57:11Z Indirect tail states formation by thermal-induced polar fluctuations in halide perovskites Wu, Bo Yuan, Haifeng Xu, Qiang Steele, Julian A. Giovanni, David Puech, Pascal Fu, Jianhui Ng, Yan Fong Nur Fadilah Jamaludin Solanki, Ankur Mhaisalkar, Subodh Mathews, Nripan Roeffaers, Maarten B. J. Grätzel, Michael Hofkens, Johan Sum, Tze Chien School of Materials Science & Engineering School of Physical and Mathematical Sciences Energy Research Institute @ NTU (ERI@N) DRNTU::Science::Physics Lasers, LEDs And Light Sources Electronic Properties And Materials Halide perovskites possess enormous potential for various optoelectronic applications. Presently, a clear understanding of the interplay between the lattice and electronic effects is still elusive. Specifically, the weakly absorbing tail states and dual emission from perovskites are not satisfactorily described by existing theories based on the Urbach tail and reabsorption effect. Herein, through temperature-dependent and time-resolved spectroscopy on metal halide perovskite single crystals with organic or inorganic A-site cations, we confirm the existence of indirect tail states below the direct transition edge to arise from a dynamical Rashba splitting effect, caused by the PbBr6 octahedral thermal polar distortions at elevated temperatures. This dynamic effect is distinct from the static Rashba splitting effect, caused by non-spherical A-site cations or surface induced lattice distortions. Our findings shed fresh perspectives on the electronic-lattice relations paramount for the design and optimization of emergent perovskites, revealing broad implications for light harvesting/photo-detection and light emission/lasing applications. NRF (Natl Research Foundation, S’pore) ASTAR (Agency for Sci., Tech. and Research, S’pore) MOE (Min. of Education, S’pore) Published version 2019-03-01T05:45:31Z 2019-12-06T17:35:18Z 2019-03-01T05:45:31Z 2019-12-06T17:35:18Z 2019 Journal Article Wu, B., Yuan, H., Xu, Q., Steele, J. A., Giovanni, D., Puech, P., . . . Sum, T. C. (2019). Indirect tail states formation by thermal-induced polar fluctuations in halide perovskites. Nature Communications, 10(1), 484-. doi:10.1038/s41467-019-08326-7 https://hdl.handle.net/10356/89862 http://hdl.handle.net/10220/47743 10.1038/s41467-019-08326-7 en Nature Communications https://doi.org/10.21979/N9/WJFNG2 © 2019 The Author(s). This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/. 10 p. application/pdf |
| spellingShingle | DRNTU::Science::Physics Lasers, LEDs And Light Sources Electronic Properties And Materials Wu, Bo Yuan, Haifeng Xu, Qiang Steele, Julian A. Giovanni, David Puech, Pascal Fu, Jianhui Ng, Yan Fong Nur Fadilah Jamaludin Solanki, Ankur Mhaisalkar, Subodh Mathews, Nripan Roeffaers, Maarten B. J. Grätzel, Michael Hofkens, Johan Sum, Tze Chien Indirect tail states formation by thermal-induced polar fluctuations in halide perovskites |
| title | Indirect tail states formation by thermal-induced polar fluctuations in halide perovskites |
| title_full | Indirect tail states formation by thermal-induced polar fluctuations in halide perovskites |
| title_fullStr | Indirect tail states formation by thermal-induced polar fluctuations in halide perovskites |
| title_full_unstemmed | Indirect tail states formation by thermal-induced polar fluctuations in halide perovskites |
| title_short | Indirect tail states formation by thermal-induced polar fluctuations in halide perovskites |
| title_sort | indirect tail states formation by thermal induced polar fluctuations in halide perovskites |
| topic | DRNTU::Science::Physics Lasers, LEDs And Light Sources Electronic Properties And Materials |
| url | https://hdl.handle.net/10356/89862 http://hdl.handle.net/10220/47743 |
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