Slow cooling and highly efficient extraction of hot carriers in colloidal perovskite nanocrystals
Hot-carrier solar cells can overcome the Shockley-Queisser limit by harvesting excess energy from hot carriers. Inorganic semiconductor nanocrystals are considered prime candidates. However, hot-carrier harvesting is compromised by competitive relaxation pathways (for example, intraband Auger proces...
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sg-ntu-dr.10356-838952021-01-14T08:21:55Z Slow cooling and highly efficient extraction of hot carriers in colloidal perovskite nanocrystals Li, Mingjie Bhaumik, Saikat Goh, Teck Wee Kumar, Muduli Subas Yantara, Natalia Grätzel, Michael Mhaisalkar, Subodh Mathews, Nripan Sum, Tze Chien School of Materials Science & Engineering School of Physical and Mathematical Sciences Energy Research Institute @ NTU (ERI@N) Organic–inorganic Nanostructures Solar Cells Hot-carrier solar cells can overcome the Shockley-Queisser limit by harvesting excess energy from hot carriers. Inorganic semiconductor nanocrystals are considered prime candidates. However, hot-carrier harvesting is compromised by competitive relaxation pathways (for example, intraband Auger process and defects) that overwhelm their phonon bottlenecks. Here we show colloidal halide perovskite nanocrystals transcend these limitations and exhibit around two orders slower hot-carrier cooling times and around four times larger hot-carrier temperatures than their bulk-film counterparts. Under low pump excitation, hot-carrier cooling mediated by a phonon bottleneck is surprisingly slower in smaller nanocrystals (contrasting with conventional nanocrystals). At high pump fluence, Auger heating dominates hot-carrier cooling, which is slower in larger nanocrystals (hitherto unobserved in conventional nanocrystals). Importantly, we demonstrate efficient room temperature hot-electrons extraction (up to ∼83%) by an energy-selective electron acceptor layer within 1 ps from surface-treated perovskite NCs thin films. These insights enable fresh approaches for extremely thin absorber and concentrator-type hot-carrier solar cells. MOE (Min. of Education, S’pore) 2017-07-13T07:36:35Z 2019-12-06T15:34:06Z 2017-07-13T07:36:35Z 2019-12-06T15:34:06Z 2017 Journal Article Li, M., Bhaumik, S., Goh, T. W., Kumar, M. S., Yantara, N., Grätzel, M., et al. (2017). Slow cooling and highly efficient extraction of hot carriers in colloidal perovskite nanocrystals. Nature Communications, 8, 14350-. 2041-1723 https://hdl.handle.net/10356/83895 http://hdl.handle.net/10220/42852 10.1038/ncomms14350 en Nature Communications © 2017 The Author(s). This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ application/pdf |
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Organic–inorganic Nanostructures Solar Cells Li, Mingjie Bhaumik, Saikat Goh, Teck Wee Kumar, Muduli Subas Yantara, Natalia Grätzel, Michael Mhaisalkar, Subodh Mathews, Nripan Sum, Tze Chien Slow cooling and highly efficient extraction of hot carriers in colloidal perovskite nanocrystals |
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Hot-carrier solar cells can overcome the Shockley-Queisser limit by harvesting excess energy from hot carriers. Inorganic semiconductor nanocrystals are considered prime candidates. However, hot-carrier harvesting is compromised by competitive relaxation pathways (for example, intraband Auger process and defects) that overwhelm their phonon bottlenecks. Here we show colloidal halide perovskite nanocrystals transcend these limitations and exhibit around two orders slower hot-carrier cooling times and around four times larger hot-carrier temperatures than their bulk-film counterparts. Under low pump excitation, hot-carrier cooling mediated by a phonon bottleneck is surprisingly slower in smaller nanocrystals (contrasting with conventional nanocrystals). At high pump fluence, Auger heating dominates hot-carrier cooling, which is slower in larger nanocrystals (hitherto unobserved in conventional nanocrystals). Importantly, we demonstrate efficient room temperature hot-electrons extraction (up to ∼83%) by an energy-selective electron acceptor layer within 1 ps from surface-treated perovskite NCs thin films. These insights enable fresh approaches for extremely thin absorber and concentrator-type hot-carrier solar cells. |
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School of Materials Science & Engineering |
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School of Materials Science & Engineering Li, Mingjie Bhaumik, Saikat Goh, Teck Wee Kumar, Muduli Subas Yantara, Natalia Grätzel, Michael Mhaisalkar, Subodh Mathews, Nripan Sum, Tze Chien |
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Article |
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Li, Mingjie Bhaumik, Saikat Goh, Teck Wee Kumar, Muduli Subas Yantara, Natalia Grätzel, Michael Mhaisalkar, Subodh Mathews, Nripan Sum, Tze Chien |
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Li, Mingjie |
title |
Slow cooling and highly efficient extraction of hot carriers in colloidal perovskite nanocrystals |
title_short |
Slow cooling and highly efficient extraction of hot carriers in colloidal perovskite nanocrystals |
title_full |
Slow cooling and highly efficient extraction of hot carriers in colloidal perovskite nanocrystals |
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Slow cooling and highly efficient extraction of hot carriers in colloidal perovskite nanocrystals |
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Slow cooling and highly efficient extraction of hot carriers in colloidal perovskite nanocrystals |
title_sort |
slow cooling and highly efficient extraction of hot carriers in colloidal perovskite nanocrystals |
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2017 |
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https://hdl.handle.net/10356/83895 http://hdl.handle.net/10220/42852 |
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1690658284849070080 |