Low threshold and efficient multiple exciton generation in halide perovskite nanocrystals
Multiple exciton generation (MEG) or carrier multiplication, a process that spawns two or more electron–hole pairs from an absorbed high-energy photon (larger than two times bandgap energy Eg), is a promising way to augment the photocurrent and overcome the Shockley–Queisser limit. Conventional semi...
| Main Authors: | , , , , , , , , , |
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| Format: | Journal Article |
| Language: | English |
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2019
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| Online Access: | https://hdl.handle.net/10356/82965 http://hdl.handle.net/10220/47527 |
| _version_ | 1826119954381930496 |
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| author | Li, Mingjie Begum, Raihana Fu, Jianhui Xu, Qiang Koh, Teck Ming Veldhuis, Sjoerd A. Grätzel, Michael Mathews, Nripan Mhaisalkar, Subodh Sum, Tze Chien |
| author2 | School of Materials Science & Engineering |
| author_facet | School of Materials Science & Engineering Li, Mingjie Begum, Raihana Fu, Jianhui Xu, Qiang Koh, Teck Ming Veldhuis, Sjoerd A. Grätzel, Michael Mathews, Nripan Mhaisalkar, Subodh Sum, Tze Chien |
| author_sort | Li, Mingjie |
| collection | NTU |
| description | Multiple exciton generation (MEG) or carrier multiplication, a process that spawns two or more electron–hole pairs from an absorbed high-energy photon (larger than two times bandgap energy Eg), is a promising way to augment the photocurrent and overcome the Shockley–Queisser limit. Conventional semiconductor nanocrystals, the forerunners, face severe challenges from fast hot-carrier cooling. Perovskite nanocrystals possess an intrinsic phonon bottleneck that prolongs slow hot-carrier cooling, transcending these limitations. Herein, we demonstrate enhanced MEG with 2.25Eg threshold and 75% slope efficiency in intermediate-confined colloidal formamidinium lead iodide nanocrystals, surpassing those in strongly confined lead sulfide or lead selenide incumbents. Efficient MEG occurs via inverse Auger process within 90 fs, afforded by the slow cooling of energetic hot carriers. These nanocrystals circumvent the conundrum over enhanced Coulombic coupling and reduced density of states in strongly confined nanocrystals. These insights may lead to the realization of next generation of solar cells and efficient optoelectronic devices. |
| first_indexed | 2024-10-01T05:08:13Z |
| format | Journal Article |
| id | ntu-10356/82965 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T05:08:13Z |
| publishDate | 2019 |
| record_format | dspace |
| spelling | ntu-10356/829652021-01-18T04:50:18Z Low threshold and efficient multiple exciton generation in halide perovskite nanocrystals Li, Mingjie Begum, Raihana Fu, Jianhui Xu, Qiang Koh, Teck Ming Veldhuis, Sjoerd A. Grätzel, Michael Mathews, Nripan Mhaisalkar, Subodh Sum, Tze Chien School of Materials Science & Engineering School of Physical and Mathematical Sciences Energy Research Institute @ NTU (ERI@N) DRNTU::Engineering::Materials Perovskite Nanocrystals Multiple Exciton Generation Multiple exciton generation (MEG) or carrier multiplication, a process that spawns two or more electron–hole pairs from an absorbed high-energy photon (larger than two times bandgap energy Eg), is a promising way to augment the photocurrent and overcome the Shockley–Queisser limit. Conventional semiconductor nanocrystals, the forerunners, face severe challenges from fast hot-carrier cooling. Perovskite nanocrystals possess an intrinsic phonon bottleneck that prolongs slow hot-carrier cooling, transcending these limitations. Herein, we demonstrate enhanced MEG with 2.25Eg threshold and 75% slope efficiency in intermediate-confined colloidal formamidinium lead iodide nanocrystals, surpassing those in strongly confined lead sulfide or lead selenide incumbents. Efficient MEG occurs via inverse Auger process within 90 fs, afforded by the slow cooling of energetic hot carriers. These nanocrystals circumvent the conundrum over enhanced Coulombic coupling and reduced density of states in strongly confined nanocrystals. These insights may lead to the realization of next generation of solar cells and efficient optoelectronic devices. NRF (Natl Research Foundation, S’pore) MOE (Min. of Education, S’pore) Published version 2019-01-21T08:51:04Z 2019-12-06T15:09:09Z 2019-01-21T08:51:04Z 2019-12-06T15:09:09Z 2018 Journal Article Li, M., Begum, R., Fu, J., Xu, Q., Koh, T. M., Veldhuis, S. A., . . . Sum, T. C. (2018). Low threshold and efficient multiple exciton generation in halide perovskite nanocrystals. Nature Communications, 9(1), 4137-. doi:10.1038/s41467-018-06596-1 https://hdl.handle.net/10356/82965 http://hdl.handle.net/10220/47527 10.1038/s41467-018-06596-1 en Nature Communications https://doi.org/10.21979/N9/HJGXR3 © 2018 The Author(s). 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/. 7 p. application/pdf |
| spellingShingle | DRNTU::Engineering::Materials Perovskite Nanocrystals Multiple Exciton Generation Li, Mingjie Begum, Raihana Fu, Jianhui Xu, Qiang Koh, Teck Ming Veldhuis, Sjoerd A. Grätzel, Michael Mathews, Nripan Mhaisalkar, Subodh Sum, Tze Chien Low threshold and efficient multiple exciton generation in halide perovskite nanocrystals |
| title | Low threshold and efficient multiple exciton generation in halide perovskite nanocrystals |
| title_full | Low threshold and efficient multiple exciton generation in halide perovskite nanocrystals |
| title_fullStr | Low threshold and efficient multiple exciton generation in halide perovskite nanocrystals |
| title_full_unstemmed | Low threshold and efficient multiple exciton generation in halide perovskite nanocrystals |
| title_short | Low threshold and efficient multiple exciton generation in halide perovskite nanocrystals |
| title_sort | low threshold and efficient multiple exciton generation in halide perovskite nanocrystals |
| topic | DRNTU::Engineering::Materials Perovskite Nanocrystals Multiple Exciton Generation |
| url | https://hdl.handle.net/10356/82965 http://hdl.handle.net/10220/47527 |
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