Broadband extrinsic self-trapped exciton emission in Sn-doped 2D lead-halide perovskites
As emerging efficient emitters, metal-halide perovskites offer the intriguing potential to the low-cost light emitting devices. However, semiconductors generally suffer from severe luminescence quenching due to insufficient confinement of excitons (bound electron-hole pairs). Here, Sn-triggered extr...
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sg-ntu-dr.10356-1445332023-07-14T15:53:34Z Broadband extrinsic self-trapped exciton emission in Sn-doped 2D lead-halide perovskites Yu, Jiancan Kong, Jintao Hao, Wei Guo, Xintong He, Huajun Leow, Wan Ru Liu, Zhiyuan Cai, Pingqiang Qian, Guodong Li, Shuzhou Chen, Xueyuan Chen, Xiaodong School of Materials Science and Engineering Innovative Centre for Flexible Devices Engineering::Materials Perovskites Sn-doping As emerging efficient emitters, metal-halide perovskites offer the intriguing potential to the low-cost light emitting devices. However, semiconductors generally suffer from severe luminescence quenching due to insufficient confinement of excitons (bound electron-hole pairs). Here, Sn-triggered extrinsic self-trapping of excitons in bulk 2D perovskite crystal, PEA2 PbI4 (PEA = phenylethylammonium), is reported, where exciton self-trapping never occurs in its pure state. By creating local potential wells, isoelectronic Sn dopants initiate the localization of excitons, which would further induce the large lattice deformation around the impurities to accommodate the self-trapped excitons. With such self-trapped states, the Sn-doped perovskites generate broadband red-to-near-infrared (NIR) emission at room temperature due to strong exciton-phonon coupling, with a remarkable quantum yield increase from 0.7% to 6.0% (8.6 folds), reaching 42.3% under a 100 mW cm-2 excitation by extrapolation. The quantum yield enhancement stems from substantial higher thermal quench activation energy of self-trapped excitons than that of free excitons (120 vs 35 meV). It is further revealed that the fast exciton diffusion involves in the initial energy transfer step by transient absorption spectroscopy. This dopant-induced extrinsic exciton self-trapping approach paves the way for extending the spectral range of perovskite emitters, and may find emerging application in efficient supercontinuum sources. Ministry of Education (MOE) Accepted version J.Y., J.K., and W.H. contributed equally to this work. The authors acknowledge the financial support from Singapore MOE (MOE2014-T2-2-140 and MOE2014-T3-1-004). The authors also thank the partial financial support from the National Natural Science Foundation of China (No. 51402259), “100 Talents Program” of Fujian Province, the Strategic Priority Research Program of the Chinese Academy of Sciences (XDB20000000), the CAS/SAFEA International Partnership Program for Creative Research Teams, and the International Postdoctoral Exchange Program. 2020-11-11T06:31:55Z 2020-11-11T06:31:55Z 2019 Journal Article Yu, J., Kong, J., Hao, W., Guo, X., He, H., Leow, W. R., . . . Chen, X. (2018). Broadband Extrinsic Self‐Trapped Exciton Emission in Sn‐Doped 2D Lead‐Halide Perovskites. Advanced Materials, 31(7), 1806385-. doi:10.1002/adma.201806385 0935-9648 https://hdl.handle.net/10356/144533 10.1002/adma.201806385 30556251 7 31 en Advanced materials This is the accepted version of the following article: Yu, J., Kong, J., Hao, W., Guo, X., He, H., Leow, W. R., . . . Chen, X. (2018). Broadband Extrinsic Self‐Trapped Exciton Emission in Sn‐Doped 2D Lead‐Halide Perovskites. Advanced Materials, 31(7), 1806385-., which has been published in final form at 10.1002/adma.201806385. This article may be used for non-commercial purposes in accordance with the Wiley Self-Archiving Policy [https://authorservices.wiley.com/authorresources/Journal-Authors/licensing/self-archiving.html]. application/pdf |
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Engineering::Materials Perovskites Sn-doping Yu, Jiancan Kong, Jintao Hao, Wei Guo, Xintong He, Huajun Leow, Wan Ru Liu, Zhiyuan Cai, Pingqiang Qian, Guodong Li, Shuzhou Chen, Xueyuan Chen, Xiaodong Broadband extrinsic self-trapped exciton emission in Sn-doped 2D lead-halide perovskites |
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As emerging efficient emitters, metal-halide perovskites offer the intriguing potential to the low-cost light emitting devices. However, semiconductors generally suffer from severe luminescence quenching due to insufficient confinement of excitons (bound electron-hole pairs). Here, Sn-triggered extrinsic self-trapping of excitons in bulk 2D perovskite crystal, PEA2 PbI4 (PEA = phenylethylammonium), is reported, where exciton self-trapping never occurs in its pure state. By creating local potential wells, isoelectronic Sn dopants initiate the localization of excitons, which would further induce the large lattice deformation around the impurities to accommodate the self-trapped excitons. With such self-trapped states, the Sn-doped perovskites generate broadband red-to-near-infrared (NIR) emission at room temperature due to strong exciton-phonon coupling, with a remarkable quantum yield increase from 0.7% to 6.0% (8.6 folds), reaching 42.3% under a 100 mW cm-2 excitation by extrapolation. The quantum yield enhancement stems from substantial higher thermal quench activation energy of self-trapped excitons than that of free excitons (120 vs 35 meV). It is further revealed that the fast exciton diffusion involves in the initial energy transfer step by transient absorption spectroscopy. This dopant-induced extrinsic exciton self-trapping approach paves the way for extending the spectral range of perovskite emitters, and may find emerging application in efficient supercontinuum sources. |
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School of Materials Science and Engineering |
author_facet |
School of Materials Science and Engineering Yu, Jiancan Kong, Jintao Hao, Wei Guo, Xintong He, Huajun Leow, Wan Ru Liu, Zhiyuan Cai, Pingqiang Qian, Guodong Li, Shuzhou Chen, Xueyuan Chen, Xiaodong |
format |
Article |
author |
Yu, Jiancan Kong, Jintao Hao, Wei Guo, Xintong He, Huajun Leow, Wan Ru Liu, Zhiyuan Cai, Pingqiang Qian, Guodong Li, Shuzhou Chen, Xueyuan Chen, Xiaodong |
author_sort |
Yu, Jiancan |
title |
Broadband extrinsic self-trapped exciton emission in Sn-doped 2D lead-halide perovskites |
title_short |
Broadband extrinsic self-trapped exciton emission in Sn-doped 2D lead-halide perovskites |
title_full |
Broadband extrinsic self-trapped exciton emission in Sn-doped 2D lead-halide perovskites |
title_fullStr |
Broadband extrinsic self-trapped exciton emission in Sn-doped 2D lead-halide perovskites |
title_full_unstemmed |
Broadband extrinsic self-trapped exciton emission in Sn-doped 2D lead-halide perovskites |
title_sort |
broadband extrinsic self-trapped exciton emission in sn-doped 2d lead-halide perovskites |
publishDate |
2020 |
url |
https://hdl.handle.net/10356/144533 |
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1772828529846648832 |