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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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Autores principales: Li, Mingjie, Bhaumik, Saikat, Goh, Teck Wee, Kumar, Muduli Subas, Yantara, Natalia, Grätzel, Michael, Mhaisalkar, Subodh, Mathews, Nripan, Sum, Tze Chien
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group 2017
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5309769/
https://www.ncbi.nlm.nih.gov/pubmed/28176882
http://dx.doi.org/10.1038/ncomms14350
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author Li, Mingjie
Bhaumik, Saikat
Goh, Teck Wee
Kumar, Muduli Subas
Yantara, Natalia
Grätzel, Michael
Mhaisalkar, Subodh
Mathews, Nripan
Sum, Tze Chien
author_facet Li, Mingjie
Bhaumik, Saikat
Goh, Teck Wee
Kumar, Muduli Subas
Yantara, Natalia
Grätzel, Michael
Mhaisalkar, Subodh
Mathews, Nripan
Sum, Tze Chien
author_sort Li, Mingjie
collection PubMed
description 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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spelling pubmed-53097692017-02-27 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 Nat Commun Article 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. Nature Publishing Group 2017-02-08 /pmc/articles/PMC5309769/ /pubmed/28176882 http://dx.doi.org/10.1038/ncomms14350 Text en Copyright © 2017, The Author(s) http://creativecommons.org/licenses/by/4.0/ 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/
spellingShingle Article
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
title 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
title_fullStr Slow cooling and highly efficient extraction of hot carriers in colloidal perovskite nanocrystals
title_full_unstemmed 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_sort slow cooling and highly efficient extraction of hot carriers in colloidal perovskite nanocrystals
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5309769/
https://www.ncbi.nlm.nih.gov/pubmed/28176882
http://dx.doi.org/10.1038/ncomms14350
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