Making and breaking of exciton cooling bottlenecks in halide perovskite nanocrystals
Harnessing quantum confinement (QC) effects in semiconductors to retard hot carrier cooling (HCC) is an attractive approach for enabling efficient hot carrier extraction to overcome the Shockley–Queisser limit. However, there is a debate about whether halide perovskite nanocrystals (PNCs) can effect...
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sg-ntu-dr.10356-1729222024-01-08T15:35:10Z Making and breaking of exciton cooling bottlenecks in halide perovskite nanocrystals Lim, Melvin Jia Wei Guo, Yuanyuan Feng, Minjun Cai, Rui Sum, Tze Chien School of Physical and Mathematical Sciences Science::Physics::Optics and light Perovskite Nanocrystals Hot Carrier Cooling Harnessing quantum confinement (QC) effects in semiconductors to retard hot carrier cooling (HCC) is an attractive approach for enabling efficient hot carrier extraction to overcome the Shockley–Queisser limit. However, there is a debate about whether halide perovskite nanocrystals (PNCs) can effectively exploit these effects. To address this, we utilized pump–probe and multipulse pump–push–probe spectroscopy to investigate HCC behavior in PNCs of varying sizes and cation compositions. Our results validate the presence of an intrinsic phonon bottleneck with clear manifestations of QC effects in small CsPbBr3 PNCs exhibiting slower HCC rates compared to those of larger PNCs. However, the replacement of inorganic Cs+ with organic cations suppresses this intrinsic bottleneck. Furthermore, PNCs exhibit distinct size-dependent HCC behavior in response to changes in the cold carrier densities. We attribute this to the enhanced exciton–exciton interactions in strongly confined PNCs that facilitate Auger heating. Importantly, our findings dispel the existing controversy and provide valuable insights into design principles for engineering QC effects in PNC hot carrier applications. LUX Photonics Consortium Ministry of Education (MOE) Nanyang Technological University National Research Foundation (NRF) Submitted/Accepted version This work is supported by the Nanyang Technological University under its NTUitive Gap Fund (NGF-2022-11-018) and the LUX Photonics Consortium Industry-IHL Collaboration Seed Grant Award (2022LUX02P01), the Ministry of Education under its AcRF Tier 2 grant (MOE-T2EP50120-0004), and the National Research Foundation (NRF) Singapore under its NRF Investigatorship (NRF-NRFI2018-04) and Competitive Research Program (CRP) (NRF-CRP25-2020-0004). 2024-01-03T06:10:59Z 2024-01-03T06:10:59Z 2023 Journal Article Lim, M. J. W., Guo, Y., Feng, M., Cai, R. & Sum, T. C. (2023). Making and breaking of exciton cooling bottlenecks in halide perovskite nanocrystals. Journal of the American Chemical Society. https://dx.doi.org/10.1021/jacs.3c09761 0002-7863 https://hdl.handle.net/10356/172922 10.1021/jacs.3c09761 en NGF-2022-11-018 2022LUX02P01 MOE-T2EP50120-0004 NRF-NRFI2018-04 NRF-CRP25-2020-0004 Journal of the American Chemical Society 10.21979/N9/IHVBEF © 2023 American Chemical Society. All rights reserved. This article may be downloaded for personal use only. Any other use requires prior permission of the copyright holder. The Version of Record is available online at http://doi.org/10.1021/jacs.3c09761. application/pdf application/pdf |
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Science::Physics::Optics and light Perovskite Nanocrystals Hot Carrier Cooling Lim, Melvin Jia Wei Guo, Yuanyuan Feng, Minjun Cai, Rui Sum, Tze Chien Making and breaking of exciton cooling bottlenecks in halide perovskite nanocrystals |
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Harnessing quantum confinement (QC) effects in semiconductors to retard hot carrier cooling (HCC) is an attractive approach for enabling efficient hot carrier extraction to overcome the Shockley–Queisser limit. However, there is a debate about whether halide perovskite nanocrystals (PNCs) can effectively exploit these effects. To address this, we utilized pump–probe and multipulse pump–push–probe spectroscopy to investigate HCC behavior in PNCs of varying sizes and cation compositions. Our results validate the presence of an intrinsic phonon bottleneck with clear manifestations of QC effects in small CsPbBr3 PNCs exhibiting slower HCC rates compared to those of larger PNCs. However, the replacement of inorganic Cs+ with organic cations suppresses this intrinsic bottleneck. Furthermore, PNCs exhibit distinct size-dependent HCC behavior in response to changes in the cold carrier densities. We attribute this to the enhanced exciton–exciton interactions in strongly confined PNCs that facilitate Auger heating. Importantly, our findings dispel the existing controversy and provide valuable insights into design principles for engineering QC effects in PNC hot carrier applications. |
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School of Physical and Mathematical Sciences |
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School of Physical and Mathematical Sciences Lim, Melvin Jia Wei Guo, Yuanyuan Feng, Minjun Cai, Rui Sum, Tze Chien |
format |
Article |
author |
Lim, Melvin Jia Wei Guo, Yuanyuan Feng, Minjun Cai, Rui Sum, Tze Chien |
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Lim, Melvin Jia Wei |
title |
Making and breaking of exciton cooling bottlenecks in halide perovskite nanocrystals |
title_short |
Making and breaking of exciton cooling bottlenecks in halide perovskite nanocrystals |
title_full |
Making and breaking of exciton cooling bottlenecks in halide perovskite nanocrystals |
title_fullStr |
Making and breaking of exciton cooling bottlenecks in halide perovskite nanocrystals |
title_full_unstemmed |
Making and breaking of exciton cooling bottlenecks in halide perovskite nanocrystals |
title_sort |
making and breaking of exciton cooling bottlenecks in halide perovskite nanocrystals |
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2024 |
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https://hdl.handle.net/10356/172922 |
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1789482975884214272 |