Dominant factors limiting the optical gain in layered two-dimensional halide perovskite thin films
Semiconductors are ubiquitous gain media for coherent light sources. Solution-processed three-dimensional (3D) halide perovskites (e.g., CH3NH3PbI3) with their outstanding room temperature optical gain properties are the latest members of this family. Their two-dimensional (2D) layered perovskite co...
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sg-ntu-dr.10356-814462022-07-12T03:02:19Z Dominant factors limiting the optical gain in layered two-dimensional halide perovskite thin films Chong, Wee Kiang Thirumal, Krishnamoorthy Giovanni, David Goh, Teck Wee Liu, Xinfeng Mathews, Nripan Mhaisalkar, Subodh Sum, Tze Chien School of Materials Science & Engineering School of Physical and Mathematical Sciences Interdisciplinary Graduate School (IGS) Research Techno Plaza Energy Research Institute @ NTU (ERI@N) Photoluminescence spectroscopy Lasing Amplified spontaneous emission Two dimensional Perovskite Semiconductors are ubiquitous gain media for coherent light sources. Solution-processed three-dimensional (3D) halide perovskites (e.g., CH3NH3PbI3) with their outstanding room temperature optical gain properties are the latest members of this family. Their two-dimensional (2D) layered perovskite counterparts with natural multiple quantum well structures exhibit strong light–matter interactions and intense excitonic luminescence. However, despite such promising traits, there have been no reports on room temperature optical gain in 2D layered perovskites. Herein, we reveal the challenges towards achieving amplified spontaneous emission (ASE) in the archetypal (C6H5C2H4NH3)2PbI4 (or PEPI) system. Temperature-dependent transient spectroscopy uncovers the dominant free exciton trapping and bound biexciton formation pathways that compete effectively with biexcitonic gain. Phenomenological rate equation modeling predicts a large biexciton ASE threshold of ∼1.4 mJ cm−2, which is beyond the damage threshold of these materials. Importantly, these findings would rationalize the difficulties in achieving optical gain in 2D perovskites and provide new insights and suggestions for overcoming these challenges. NRF (Natl Research Foundation, S’pore) MOE (Min. of Education, S’pore) ASTAR (Agency for Sci., Tech. and Research, S’pore) Published version 2016-06-27T05:03:18Z 2019-12-06T14:31:09Z 2016-06-27T05:03:18Z 2019-12-06T14:31:09Z 2016 2016 Journal Article Chong, W. K., Thirumal, K., Giovanni, D., Goh, T. W., Liu, X., Mathews, N., . . . Sum, T. C. (2016). Dominant factors limiting the optical gain in layered two-dimensional halide perovskite thin films. Physical Chemistry Chemical Physics, 21(18), 14701-14708. doi: 10.1039/C6CP01955B 1463-9076 https://hdl.handle.net/10356/81446 http://hdl.handle.net/10220/40797 10.1039/C6CP01955B 194876 en Physical Chemistry Chemical Physics https://doi.org/10.21979/N9/WJSVVC © 2016 The Author(s) (Royal Society of Chemistry). This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. 8 p. application/pdf |
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Photoluminescence spectroscopy Lasing Amplified spontaneous emission Two dimensional Perovskite |
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Photoluminescence spectroscopy Lasing Amplified spontaneous emission Two dimensional Perovskite Chong, Wee Kiang Thirumal, Krishnamoorthy Giovanni, David Goh, Teck Wee Liu, Xinfeng Mathews, Nripan Mhaisalkar, Subodh Sum, Tze Chien Dominant factors limiting the optical gain in layered two-dimensional halide perovskite thin films |
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Semiconductors are ubiquitous gain media for coherent light sources. Solution-processed three-dimensional (3D) halide perovskites (e.g., CH3NH3PbI3) with their outstanding room temperature optical gain properties are the latest members of this family. Their two-dimensional (2D) layered perovskite counterparts with natural multiple quantum well structures exhibit strong light–matter interactions and intense excitonic luminescence. However, despite such promising traits, there have been no reports on room temperature optical gain in 2D layered perovskites. Herein, we reveal the challenges towards achieving amplified spontaneous emission (ASE) in the archetypal (C6H5C2H4NH3)2PbI4 (or PEPI) system. Temperature-dependent transient spectroscopy uncovers the dominant free exciton trapping and bound biexciton formation pathways that compete effectively with biexcitonic gain. Phenomenological rate equation modeling predicts a large biexciton ASE threshold of ∼1.4 mJ cm−2, which is beyond the damage threshold of these materials. Importantly, these findings would rationalize the difficulties in achieving optical gain in 2D perovskites and provide new insights and suggestions for overcoming these challenges. |
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School of Materials Science & Engineering |
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School of Materials Science & Engineering Chong, Wee Kiang Thirumal, Krishnamoorthy Giovanni, David Goh, Teck Wee Liu, Xinfeng Mathews, Nripan Mhaisalkar, Subodh Sum, Tze Chien |
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Chong, Wee Kiang Thirumal, Krishnamoorthy Giovanni, David Goh, Teck Wee Liu, Xinfeng Mathews, Nripan Mhaisalkar, Subodh Sum, Tze Chien |
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Chong, Wee Kiang |
title |
Dominant factors limiting the optical gain in layered two-dimensional halide perovskite thin films |
title_short |
Dominant factors limiting the optical gain in layered two-dimensional halide perovskite thin films |
title_full |
Dominant factors limiting the optical gain in layered two-dimensional halide perovskite thin films |
title_fullStr |
Dominant factors limiting the optical gain in layered two-dimensional halide perovskite thin films |
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Dominant factors limiting the optical gain in layered two-dimensional halide perovskite thin films |
title_sort |
dominant factors limiting the optical gain in layered two-dimensional halide perovskite thin films |
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2016 |
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https://hdl.handle.net/10356/81446 http://hdl.handle.net/10220/40797 https://doi.org/10.21979/N9/WJSVVC |
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