Ultrahigh-efficiency aqueous flat nanocrystals of CdSe/CdS@Cd1−xZnxS colloidal core/crown@alloyed-shell quantum wells
Colloidal semiconductor nanoplatelets (NPLs) are highly promising luminescent materials owing to their exceptionally narrow emission spectra. While high-efficiency NPLs in non-polar organic media can be obtained readily, NPLs in aqueous media suffer from extremely low quantum yields (QYs), which com...
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sg-ntu-dr.10356-1423282021-05-01T20:12:08Z Ultrahigh-efficiency aqueous flat nanocrystals of CdSe/CdS@Cd1−xZnxS colloidal core/crown@alloyed-shell quantum wells Shendre, Sushant Delikanli, Savas Li, Mingjie Dede, Didem Pan, Zhenying Ha, Son Tung Fu, Yuan Hsing Hernández-Martínez, Pedro L. Yu, Junhong Erdem, Onur Kuznetsov, Arseniy I. Dang, Cuong Sum, Tze Chien Demir, Hilmi Volkan School of Electrical and Electronic Engineering School of Physical and Mathematical Sciences LUMINOUS! Centre of Excellence for Semiconductor Lighting and Displays Research Techno Plaza Engineering::Electrical and electronic engineering Nanoplatelets Colloidal Quantum Wells Colloidal semiconductor nanoplatelets (NPLs) are highly promising luminescent materials owing to their exceptionally narrow emission spectra. While high-efficiency NPLs in non-polar organic media can be obtained readily, NPLs in aqueous media suffer from extremely low quantum yields (QYs), which completely undermines their potential, especially in biological applications. Here, we show high-efficiency water-soluble CdSe/CdS@Cd1−xZnxS core/crown@shell NPLs formed by layer-by-layer grown and composition-tuned gradient Cd1−xZnxS shells on CdSe/CdS core/crown seeds. Such control of shell composition with monolayer precision and effective peripheral crown passivation, together with the compact capping density of short 3-mercaptopropionic acid ligands, allow for QYs reaching 90% in water, accompanied by a significantly increased photoluminescence lifetime (∼35 ns), indicating the suppression of nonradiative channels in these NPLs. We also demonstrate the controlled attachment of these NPLs without stacking at the nanoscale by taking advantage of their 2D geometry and hydrophilicity. This is a significant step in achieving controlled assemblies and overcoming the stacking process, which otherwise undermines their film formation and performance in optoelectronic applications. Moreover, we show that the parallel orientation of such NPLs achieved by the controlled attachment enables directed emission perpendicular to the surface of the NPL films, which is highly advantageous for light extraction in light-emitting platforms. NRF (Natl Research Foundation, S’pore) ASTAR (Agency for Sci., Tech. and Research, S’pore) MOE (Min. of Education, S’pore) Accepted version 2020-06-19T04:26:12Z 2020-06-19T04:26:12Z 2018 Journal Article Shendre, S., Delikanli, S., Li, M., Dede, D., Pan, Z., Ha, S. T., . . . Demir, H. V. (2019). Ultrahigh-efficiency aqueous flat nanocrystals of CdSe/CdS@Cd1−xZnxS colloidal core/crown@alloyed-shell quantum wells. Nanoscale, 11(1), 301–310. doi:10.1039/C8NR07879C 2040-3364 https://hdl.handle.net/10356/142328 10.1039/C8NR07879C 1 11 301 310 en Nanoscale © 2019 The Royal Society of Chemistry. All rights reserved. This paper was published in Nanoscale and is made available with permission of The Royal Society of Chemistry. application/pdf |
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Engineering::Electrical and electronic engineering Nanoplatelets Colloidal Quantum Wells |
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Engineering::Electrical and electronic engineering Nanoplatelets Colloidal Quantum Wells Shendre, Sushant Delikanli, Savas Li, Mingjie Dede, Didem Pan, Zhenying Ha, Son Tung Fu, Yuan Hsing Hernández-Martínez, Pedro L. Yu, Junhong Erdem, Onur Kuznetsov, Arseniy I. Dang, Cuong Sum, Tze Chien Demir, Hilmi Volkan Ultrahigh-efficiency aqueous flat nanocrystals of CdSe/CdS@Cd1−xZnxS colloidal core/crown@alloyed-shell quantum wells |
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Colloidal semiconductor nanoplatelets (NPLs) are highly promising luminescent materials owing to their exceptionally narrow emission spectra. While high-efficiency NPLs in non-polar organic media can be obtained readily, NPLs in aqueous media suffer from extremely low quantum yields (QYs), which completely undermines their potential, especially in biological applications. Here, we show high-efficiency water-soluble CdSe/CdS@Cd1−xZnxS core/crown@shell NPLs formed by layer-by-layer grown and composition-tuned gradient Cd1−xZnxS shells on CdSe/CdS core/crown seeds. Such control of shell composition with monolayer precision and effective peripheral crown passivation, together with the compact capping density of short 3-mercaptopropionic acid ligands, allow for QYs reaching 90% in water, accompanied by a significantly increased photoluminescence lifetime (∼35 ns), indicating the suppression of nonradiative channels in these NPLs. We also demonstrate the controlled attachment of these NPLs without stacking at the nanoscale by taking advantage of their 2D geometry and hydrophilicity. This is a significant step in achieving controlled assemblies and overcoming the stacking process, which otherwise undermines their film formation and performance in optoelectronic applications. Moreover, we show that the parallel orientation of such NPLs achieved by the controlled attachment enables directed emission perpendicular to the surface of the NPL films, which is highly advantageous for light extraction in light-emitting platforms. |
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School of Electrical and Electronic Engineering |
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School of Electrical and Electronic Engineering Shendre, Sushant Delikanli, Savas Li, Mingjie Dede, Didem Pan, Zhenying Ha, Son Tung Fu, Yuan Hsing Hernández-Martínez, Pedro L. Yu, Junhong Erdem, Onur Kuznetsov, Arseniy I. Dang, Cuong Sum, Tze Chien Demir, Hilmi Volkan |
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Article |
author |
Shendre, Sushant Delikanli, Savas Li, Mingjie Dede, Didem Pan, Zhenying Ha, Son Tung Fu, Yuan Hsing Hernández-Martínez, Pedro L. Yu, Junhong Erdem, Onur Kuznetsov, Arseniy I. Dang, Cuong Sum, Tze Chien Demir, Hilmi Volkan |
author_sort |
Shendre, Sushant |
title |
Ultrahigh-efficiency aqueous flat nanocrystals of CdSe/CdS@Cd1−xZnxS colloidal core/crown@alloyed-shell quantum wells |
title_short |
Ultrahigh-efficiency aqueous flat nanocrystals of CdSe/CdS@Cd1−xZnxS colloidal core/crown@alloyed-shell quantum wells |
title_full |
Ultrahigh-efficiency aqueous flat nanocrystals of CdSe/CdS@Cd1−xZnxS colloidal core/crown@alloyed-shell quantum wells |
title_fullStr |
Ultrahigh-efficiency aqueous flat nanocrystals of CdSe/CdS@Cd1−xZnxS colloidal core/crown@alloyed-shell quantum wells |
title_full_unstemmed |
Ultrahigh-efficiency aqueous flat nanocrystals of CdSe/CdS@Cd1−xZnxS colloidal core/crown@alloyed-shell quantum wells |
title_sort |
ultrahigh-efficiency aqueous flat nanocrystals of cdse/cds@cd1−xznxs colloidal core/crown@alloyed-shell quantum wells |
publishDate |
2020 |
url |
https://hdl.handle.net/10356/142328 |
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1698713680981524480 |