Origins of the long-range exciton diffusion in perovskite nanocrystal films : photon recycling vs exciton hopping

The outstanding optoelectronic performance of lead halide perovskites lies in their exceptional carrier diffusion properties. As the perovskite material dimensionality is reduced to exploit the quantum confinement effects, the disruption to the perovskite lattice, often with insulating organic ligan...

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Main Authors: Giovanni, David, Righetto, Marcello, Zhang, Qiannan, Lim, Melvin Jia Wei, Ramesh, Sankaran, Sum, Tze Chien
Other Authors: School of Physical and Mathematical Sciences
Format: Article
Language:English
Published: 2021
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Online Access:https://hdl.handle.net/10356/145997
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Institution: Nanyang Technological University
Language: English
id sg-ntu-dr.10356-145997
record_format dspace
institution Nanyang Technological University
building NTU Library
continent Asia
country Singapore
Singapore
content_provider NTU Library
collection DR-NTU
language English
topic Science::Physics
Electronics, Photonics and Device Physics
Micro-optics
spellingShingle Science::Physics
Electronics, Photonics and Device Physics
Micro-optics
Giovanni, David
Righetto, Marcello
Zhang, Qiannan
Lim, Melvin Jia Wei
Ramesh, Sankaran
Sum, Tze Chien
Origins of the long-range exciton diffusion in perovskite nanocrystal films : photon recycling vs exciton hopping
description The outstanding optoelectronic performance of lead halide perovskites lies in their exceptional carrier diffusion properties. As the perovskite material dimensionality is reduced to exploit the quantum confinement effects, the disruption to the perovskite lattice, often with insulating organic ligands, raises new questions on the charge diffusion properties. Herein, we report direct imaging of >1 μm exciton diffusion lengths in CH3NH3PbBr3 perovskite nanocrystal (PNC) films. Surprisingly, the resulting exciton mobilities in these PNC films can reach 10 ± 2 cm2 V-1 s-1, which is counterintuitively several times higher than the carrier mobility in 3D perovskite films. We show that this ultralong exciton diffusion originates from both efficient inter-NC exciton hopping (via Förster energy transfer) and the photon recycling process with a smaller yet significant contribution. Importantly, our study not only sheds new light on the highly debated origins of the excellent exciton diffusion in PNC films but also highlights the potential of PNCs for optoelectronic applications.
author2 School of Physical and Mathematical Sciences
author_facet School of Physical and Mathematical Sciences
Giovanni, David
Righetto, Marcello
Zhang, Qiannan
Lim, Melvin Jia Wei
Ramesh, Sankaran
Sum, Tze Chien
format Article
author Giovanni, David
Righetto, Marcello
Zhang, Qiannan
Lim, Melvin Jia Wei
Ramesh, Sankaran
Sum, Tze Chien
author_sort Giovanni, David
title Origins of the long-range exciton diffusion in perovskite nanocrystal films : photon recycling vs exciton hopping
title_short Origins of the long-range exciton diffusion in perovskite nanocrystal films : photon recycling vs exciton hopping
title_full Origins of the long-range exciton diffusion in perovskite nanocrystal films : photon recycling vs exciton hopping
title_fullStr Origins of the long-range exciton diffusion in perovskite nanocrystal films : photon recycling vs exciton hopping
title_full_unstemmed Origins of the long-range exciton diffusion in perovskite nanocrystal films : photon recycling vs exciton hopping
title_sort origins of the long-range exciton diffusion in perovskite nanocrystal films : photon recycling vs exciton hopping
publishDate 2021
url https://hdl.handle.net/10356/145997
_version_ 1759857873279516672
spelling sg-ntu-dr.10356-1459972023-02-28T19:27:30Z Origins of the long-range exciton diffusion in perovskite nanocrystal films : photon recycling vs exciton hopping Giovanni, David Righetto, Marcello Zhang, Qiannan Lim, Melvin Jia Wei Ramesh, Sankaran Sum, Tze Chien School of Physical and Mathematical Sciences Interdisciplinary Graduate School (IGS) Energy Research Institute @ NTU (ERI@N) Science::Physics Electronics, Photonics and Device Physics Micro-optics The outstanding optoelectronic performance of lead halide perovskites lies in their exceptional carrier diffusion properties. As the perovskite material dimensionality is reduced to exploit the quantum confinement effects, the disruption to the perovskite lattice, often with insulating organic ligands, raises new questions on the charge diffusion properties. Herein, we report direct imaging of >1 μm exciton diffusion lengths in CH3NH3PbBr3 perovskite nanocrystal (PNC) films. Surprisingly, the resulting exciton mobilities in these PNC films can reach 10 ± 2 cm2 V-1 s-1, which is counterintuitively several times higher than the carrier mobility in 3D perovskite films. We show that this ultralong exciton diffusion originates from both efficient inter-NC exciton hopping (via Förster energy transfer) and the photon recycling process with a smaller yet significant contribution. Importantly, our study not only sheds new light on the highly debated origins of the excellent exciton diffusion in PNC films but also highlights the potential of PNCs for optoelectronic applications. Ministry of Education (MOE) National Research Foundation (NRF) Published version We acknowledged Dr. Pio John S. Buenconsejo from the Facility for Analysis Characterization Testing and Simulation (FACTS), Nanyang Technological University, Singapore, for help with GISAXS measurements. This research/project was supported by Nanyang Technological University under its start-up grants (M4080514, M4081630); the Ministry of Education under its AcRF Tier 1 grant (RG91/19) and Tier 2 grants (MOE2016-T2-1-034, MOE2017-T2-1-001, and MOE2017-T2-2-002); and the National Research Foundation (NRF) Singapore under its NRF Investigatorship (NRF-NRFI-2018-04) and Competitive Research Programme (NRF-CRP14-2014-03). Author information Author notes These authors contributed equally: David Giovanni, Marcello Righetto Affiliations Division of Physics and Applied Physics, School of Physical and Mathematical Sciences, Nanyang Technological University (NTU), 21 Nanyang Link, Singapore, 637371, Singapore David Giovanni, Marcello Righetto, Qiannan Zhang, Jia Wei Melvin Lim, Sankaran Ramesh & Tze Chien Sum Energy Research Institute @NTU (ERI@N), Interdisciplinary Graduate School, Nanyang Technological University, 50 Nanyang Avenue, S2-B3a-01, Singapore, 639798, Singapore Jia Wei Melvin Lim & Sankaran Ramesh Contributions D.G. and M.R. conceived the idea. M.R. synthesized the samples. D.G. and M.R. performed the optical spectroscopy measurements and analysis of perovskite samples. Q.N. performed the AFM and GISAXS measurements and analysis. M.R. and J.W.M.L. performed the TEM measurement and analysis. D.G. and S.R. performed CdSe sample fabrication and measurement. T.C.S. led the project. All authors were involved in writing the manuscript. Corresponding author Correspondence to Tze Chien Sum. Ethics declarations Conflict of interest The authors declare that they have no conflict of interest. Supplementary information Supplementary Information for Origins of the Long-Range Exciton Diffusion in Perovskite Nanocrystal Films: Photon Recycling vs Exciton Hopping Rights and permissions Open Access 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/. Reprints and Permissions About this article Verify currency and authenticity via CrossMark Cite this article Giovanni, D., Righetto, M., Zhang, Q. et al. Origins of the long-range exciton diffusion in perovskite nanocrystal films: photon recycling vs exciton hopping. Light Sci Appl 10, 2 (2021). https://doi.org/10.1038/s41377-020-00443-z Download citation Received19 July 2020 Revised13 November 2020 Accepted23 November 2020 Published01 January 2021 DOIhttps://doi.org/10.1038/s41377-020-00443-z Share this article Anyone you share the following link with will be able to read this content: 2021-01-20T02:58:07Z 2021-01-20T02:58:07Z 2021 Journal Article Giovanni, D., Righetto, M., Zhang, Q., Lim, M. J. W., Ramesh, S., & Sum, T. C. (2021). Origins of the long-range exciton diffusion in perovskite nanocrystal films: photon recycling vs exciton hopping. Light: Science & Applications, 10(1), 2-. https://doi.org/10.1038/s41377-020-00443-z 2047-7538 0000-0002-2764-5613 0000-0001-5507-1445 0000-0002-8139-6160 0000-0001-6284-2340 0000-0003-4049-2719 https://hdl.handle.net/10356/145997 10.1038/s41377-020-00443-z 33386385 2-s2.0-85098562466 10 en M4080514 M4081630 RG91/19 MOE2016-T2-1-034 MOE2017-T2-1-001 MOE2017-T2-2-002 NRF-NRFI-2018-04 NRF-CRP14-2014-03 Light, science & applications 10.21979/N9/6QTW2E © 2021 The Author(s). This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution andreproductionin any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a linktotheCreativeCommons license,and indicate ifchanges were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicatedotherwise in a credit line to the material. Ifmaterial 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 obtainpermission directly from the copyright holder. To view a copy of this license, visithttp://creativecommons.org/licenses/by/4.0/. application/pdf