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Understanding the Optoelectronic Processes in Colloidal 2D Multi‐Layered MAPbBr<sub>3</sub> Perovskite Nanosheets: Funneling, Recombination and Self‐Trapped Excitons

André Niebur, Eugen Klein, Rostyslav Lesyuk, Christian Klinke, Jannika Lauth Orcid Logo

Advanced Optical Materials, Volume: 13, Issue: 12

Swansea University Author: Christian Klinke

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DOI (Published version): 10.1002/adom.202402923

Abstract

Colloidal chemistry methods have made quasi 2D perovskites readily accessible. Ultrathin perovskites exhibit charge transport properties which are beneficial for solar cells and the combination of layers with different thicknesses directs charge carriers toward thicker layers with a smaller bandgap....

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Published in: Advanced Optical Materials
ISSN: 2195-1071 2195-1071
Published: Wiley 2025
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URI: https://cronfa.swan.ac.uk/Record/cronfa69416
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spelling 2025-05-02T16:00:58.0478450 v2 69416 2025-05-02 Understanding the Optoelectronic Processes in Colloidal 2D Multi‐Layered MAPbBr<sub>3</sub> Perovskite Nanosheets: Funneling, Recombination and Self‐Trapped Excitons c10c44238eabfb203111f88a965f5372 Christian Klinke Christian Klinke true false 2025-05-02 Colloidal chemistry methods have made quasi 2D perovskites readily accessible. Ultrathin perovskites exhibit charge transport properties which are beneficial for solar cells and the combination of layers with different thicknesses directs charge carriers toward thicker layers with a smaller bandgap. However, detailed knowledge about the mechanisms by which excitons and charge carriers funnel and recombine in these structures is lacking. Here, colloidal 2D methylammonium lead bromide (MAPbBr3) Ruddlesden-Popper perovskites with a broad combination of layers (n = 3 to 10, and bulk fractions with n > 10) is characterized by femtosecond transient absorption spectroscopy and time-resolved photoluminescence. It is found that second- and third-order processes dominate in MAPbBr3 nanosheets, indicating exciton-exciton annihilation (EEA) and Auger recombination. Long-lived excitons in thin layers (e.g., n  =  5, Eb =  136 meV) funnel into high n within 10–50 ps, which decreases their exciton binding energy below kBT and leads to radiative recombination. Parallel and consecutive funneling compete with trapping processes, making funneling an excellent tool to overcome exciton self-trapping when high-quality n-n interfaces are present. Free charge carriers in high-n regions on the other hand facilitate radiative recombination and EEA is bypassed, which is desirable for LED and lasing applications. Journal Article Advanced Optical Materials 13 12 Wiley 2195-1071 2195-1071 CH3NH3PbBr3; Elliott theory; excitons; femtosecond transient absorption spectroscopy; layered perovskites; trapping 23 4 2025 2025-04-23 10.1002/adom.202402923 COLLEGE NANME COLLEGE CODE Swansea University Other Bundesministerium für Bildung und Forschung. Grant Number: Athene Grant Niedersächsische Ministerium für Wissenschaft und Kultur. Grant Number: Stay-3/22-7633/2022 Deutsche Forschungsgemeinschaft. Grant Number: SFB1477-441234705,INST264/188-1FUGG,INST264/161-1FUGG,EXC2122ProjectID390833453,INST37/1160-1FUGG European Regional Development Fund. Grant Numbers: GHS-20-0035/P000376218, GHS-20-0036/P000379642 2025-05-02T16:00:58.0478450 2025-05-02T15:54:30.7309795 Faculty of Science and Engineering School of Engineering and Applied Sciences - Chemistry André Niebur 1 Eugen Klein 2 Rostyslav Lesyuk 3 Christian Klinke 4 Jannika Lauth 0000-0002-6054-9615 5 69416__34178__932716a5c3224350930d25267e1e1fe1.pdf 69416.VoR.pdf 2025-05-02T15:58:17.9522086 Output 3288905 application/pdf Version of Record true © 2025 The Author(s). This is an open access article under the terms of the Creative Commons Attribution License. true eng http://creativecommons.org/licenses/by/4.0/
title Understanding the Optoelectronic Processes in Colloidal 2D Multi‐Layered MAPbBr<sub>3</sub> Perovskite Nanosheets: Funneling, Recombination and Self‐Trapped Excitons
spellingShingle Understanding the Optoelectronic Processes in Colloidal 2D Multi‐Layered MAPbBr<sub>3</sub> Perovskite Nanosheets: Funneling, Recombination and Self‐Trapped Excitons
Christian Klinke
title_short Understanding the Optoelectronic Processes in Colloidal 2D Multi‐Layered MAPbBr<sub>3</sub> Perovskite Nanosheets: Funneling, Recombination and Self‐Trapped Excitons
title_full Understanding the Optoelectronic Processes in Colloidal 2D Multi‐Layered MAPbBr<sub>3</sub> Perovskite Nanosheets: Funneling, Recombination and Self‐Trapped Excitons
title_fullStr Understanding the Optoelectronic Processes in Colloidal 2D Multi‐Layered MAPbBr<sub>3</sub> Perovskite Nanosheets: Funneling, Recombination and Self‐Trapped Excitons
title_full_unstemmed Understanding the Optoelectronic Processes in Colloidal 2D Multi‐Layered MAPbBr<sub>3</sub> Perovskite Nanosheets: Funneling, Recombination and Self‐Trapped Excitons
title_sort Understanding the Optoelectronic Processes in Colloidal 2D Multi‐Layered MAPbBr<sub>3</sub> Perovskite Nanosheets: Funneling, Recombination and Self‐Trapped Excitons
author_id_str_mv c10c44238eabfb203111f88a965f5372
author_id_fullname_str_mv c10c44238eabfb203111f88a965f5372_***_Christian Klinke
author Christian Klinke
author2 André Niebur
Eugen Klein
Rostyslav Lesyuk
Christian Klinke
Jannika Lauth
format Journal article
container_title Advanced Optical Materials
container_volume 13
container_issue 12
publishDate 2025
institution Swansea University
issn 2195-1071
2195-1071
doi_str_mv 10.1002/adom.202402923
publisher Wiley
college_str Faculty of Science and Engineering
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hierarchy_top_id facultyofscienceandengineering
hierarchy_top_title Faculty of Science and Engineering
hierarchy_parent_id facultyofscienceandengineering
hierarchy_parent_title Faculty of Science and Engineering
department_str School of Engineering and Applied Sciences - Chemistry{{{_:::_}}}Faculty of Science and Engineering{{{_:::_}}}School of Engineering and Applied Sciences - Chemistry
document_store_str 1
active_str 0
description Colloidal chemistry methods have made quasi 2D perovskites readily accessible. Ultrathin perovskites exhibit charge transport properties which are beneficial for solar cells and the combination of layers with different thicknesses directs charge carriers toward thicker layers with a smaller bandgap. However, detailed knowledge about the mechanisms by which excitons and charge carriers funnel and recombine in these structures is lacking. Here, colloidal 2D methylammonium lead bromide (MAPbBr3) Ruddlesden-Popper perovskites with a broad combination of layers (n = 3 to 10, and bulk fractions with n > 10) is characterized by femtosecond transient absorption spectroscopy and time-resolved photoluminescence. It is found that second- and third-order processes dominate in MAPbBr3 nanosheets, indicating exciton-exciton annihilation (EEA) and Auger recombination. Long-lived excitons in thin layers (e.g., n  =  5, Eb =  136 meV) funnel into high n within 10–50 ps, which decreases their exciton binding energy below kBT and leads to radiative recombination. Parallel and consecutive funneling compete with trapping processes, making funneling an excellent tool to overcome exciton self-trapping when high-quality n-n interfaces are present. Free charge carriers in high-n regions on the other hand facilitate radiative recombination and EEA is bypassed, which is desirable for LED and lasing applications.
published_date 2025-04-23T05:29:33Z
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