Energetic disorder dominates optical properties and recombination dynamics in tin-lead perovskite nanocrystals

Tin-lead alloyed perovskite nanocrystals (PNCs) offer a promising pathway toward low-toxicity and air-stable light-emitting devices. However, substantial energetic disorder has thus far hindered their lighting applications compared to pure lead-based PNCs. A fundamental understanding of this disorde...

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Main Authors: Dandan Wang, Yusheng Li, Yongge Yang, Chao Ding, Yuyao Wei, Dong Liu, Hua Li, Huan Bi, Shikai Chen, Sujun Ji, Boyu Zhang, Yao Guo, Huiyun Wei, Hongshi Li, Shuzi Hayase, Qing Shen
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Language:English
Published: KeAi Communications Co. Ltd. 2025-01-01
Series:eScience
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Online Access:http://www.sciencedirect.com/science/article/pii/S2667141724000636
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author Dandan Wang
Yusheng Li
Yongge Yang
Chao Ding
Yuyao Wei
Dong Liu
Hua Li
Huan Bi
Shikai Chen
Sujun Ji
Boyu Zhang
Yao Guo
Huiyun Wei
Hongshi Li
Shuzi Hayase
Qing Shen
author_facet Dandan Wang
Yusheng Li
Yongge Yang
Chao Ding
Yuyao Wei
Dong Liu
Hua Li
Huan Bi
Shikai Chen
Sujun Ji
Boyu Zhang
Yao Guo
Huiyun Wei
Hongshi Li
Shuzi Hayase
Qing Shen
author_sort Dandan Wang
collection DOAJ
description Tin-lead alloyed perovskite nanocrystals (PNCs) offer a promising pathway toward low-toxicity and air-stable light-emitting devices. However, substantial energetic disorder has thus far hindered their lighting applications compared to pure lead-based PNCs. A fundamental understanding of this disorder and its impact on optical properties is crucial for overcoming this limitation. Here, using temperature-dependent static and transient absorption spectroscopy, we meticulously distinguish the contributions of static disorder (including defects, impurities, etc.) and dynamic disorder (carrier–phonon interactions). We reveal how these disorders shape band-tail structure and ultimately influence inter-band carrier recombination behaviors. Surprisingly, we find that static and dynamic disorder primarily control band-tail defect states and bandgap renormalization, respectively, which together modulate fast carrier trapping and slow band-band recombination rates. Furthermore, we link these disorders to the tin-induced symmetry-lowering distortions in tin-lead alloyed PNCs. These findings illuminate critical design principles for highly luminescent, low-toxicity tin-lead PNCs, accelerating their adoption in optoelectronic applications.
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language English
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publisher KeAi Communications Co. Ltd.
record_format Article
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spelling doaj-art-c6fe8fe9e5d2448f8abc269ab8370f052025-01-04T04:57:21ZengKeAi Communications Co. Ltd.eScience2667-14172025-01-0151100279Energetic disorder dominates optical properties and recombination dynamics in tin-lead perovskite nanocrystalsDandan Wang0Yusheng Li1Yongge Yang2Chao Ding3Yuyao Wei4Dong Liu5Hua Li6Huan Bi7Shikai Chen8Sujun Ji9Boyu Zhang10Yao Guo11Huiyun Wei12Hongshi Li13Shuzi Hayase14Qing Shen15Faculty of Informatics and Engineering, The University of Electro-Communications, 1-5-1 Chofugaoka, Chofu, Tokyo 182-8585, JapanFaculty of Informatics and Engineering, The University of Electro-Communications, 1-5-1 Chofugaoka, Chofu, Tokyo 182-8585, Japan; Corresponding authors.Faculty of Informatics and Engineering, The University of Electro-Communications, 1-5-1 Chofugaoka, Chofu, Tokyo 182-8585, JapanFaculty of Informatics and Engineering, The University of Electro-Communications, 1-5-1 Chofugaoka, Chofu, Tokyo 182-8585, JapanFaculty of Informatics and Engineering, The University of Electro-Communications, 1-5-1 Chofugaoka, Chofu, Tokyo 182-8585, JapanFaculty of Informatics and Engineering, The University of Electro-Communications, 1-5-1 Chofugaoka, Chofu, Tokyo 182-8585, JapanFaculty of Informatics and Engineering, The University of Electro-Communications, 1-5-1 Chofugaoka, Chofu, Tokyo 182-8585, JapanFaculty of Informatics and Engineering, The University of Electro-Communications, 1-5-1 Chofugaoka, Chofu, Tokyo 182-8585, JapanFaculty of Informatics and Engineering, The University of Electro-Communications, 1-5-1 Chofugaoka, Chofu, Tokyo 182-8585, JapanFaculty of Informatics and Engineering, The University of Electro-Communications, 1-5-1 Chofugaoka, Chofu, Tokyo 182-8585, JapanFaculty of Informatics and Engineering, The University of Electro-Communications, 1-5-1 Chofugaoka, Chofu, Tokyo 182-8585, JapanSchool of Materials Science and Engineering, Henan Joint International Research Laboratory of Nanocomposite Sensing Materials, Anyang Institute of Technology, Anyang 455000, ChinaSchool of Mathematics and Physics, University of Science and Technology Beijing, Beijing 100083, ChinaInstitute of New Energy Materials Chemistry, School of Materials Science and Engineering, Nankai University, Tianjin 300350, Chinai-Powered Energy System Research Center (i-PERC), The University of Electro-Communications, 1-5-1 Chofugaoka, Chofu, Tokyo 182-8585, JapanFaculty of Informatics and Engineering, The University of Electro-Communications, 1-5-1 Chofugaoka, Chofu, Tokyo 182-8585, Japan; Corresponding authors.Tin-lead alloyed perovskite nanocrystals (PNCs) offer a promising pathway toward low-toxicity and air-stable light-emitting devices. However, substantial energetic disorder has thus far hindered their lighting applications compared to pure lead-based PNCs. A fundamental understanding of this disorder and its impact on optical properties is crucial for overcoming this limitation. Here, using temperature-dependent static and transient absorption spectroscopy, we meticulously distinguish the contributions of static disorder (including defects, impurities, etc.) and dynamic disorder (carrier–phonon interactions). We reveal how these disorders shape band-tail structure and ultimately influence inter-band carrier recombination behaviors. Surprisingly, we find that static and dynamic disorder primarily control band-tail defect states and bandgap renormalization, respectively, which together modulate fast carrier trapping and slow band-band recombination rates. Furthermore, we link these disorders to the tin-induced symmetry-lowering distortions in tin-lead alloyed PNCs. These findings illuminate critical design principles for highly luminescent, low-toxicity tin-lead PNCs, accelerating their adoption in optoelectronic applications.http://www.sciencedirect.com/science/article/pii/S2667141724000636Tin-lead alloyedPerovskite nanocrystalsEnergetic disorderBand-tail structureCarrier recombination
spellingShingle Dandan Wang
Yusheng Li
Yongge Yang
Chao Ding
Yuyao Wei
Dong Liu
Hua Li
Huan Bi
Shikai Chen
Sujun Ji
Boyu Zhang
Yao Guo
Huiyun Wei
Hongshi Li
Shuzi Hayase
Qing Shen
Energetic disorder dominates optical properties and recombination dynamics in tin-lead perovskite nanocrystals
eScience
Tin-lead alloyed
Perovskite nanocrystals
Energetic disorder
Band-tail structure
Carrier recombination
title Energetic disorder dominates optical properties and recombination dynamics in tin-lead perovskite nanocrystals
title_full Energetic disorder dominates optical properties and recombination dynamics in tin-lead perovskite nanocrystals
title_fullStr Energetic disorder dominates optical properties and recombination dynamics in tin-lead perovskite nanocrystals
title_full_unstemmed Energetic disorder dominates optical properties and recombination dynamics in tin-lead perovskite nanocrystals
title_short Energetic disorder dominates optical properties and recombination dynamics in tin-lead perovskite nanocrystals
title_sort energetic disorder dominates optical properties and recombination dynamics in tin lead perovskite nanocrystals
topic Tin-lead alloyed
Perovskite nanocrystals
Energetic disorder
Band-tail structure
Carrier recombination
url http://www.sciencedirect.com/science/article/pii/S2667141724000636
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