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Quantum Dot Self‐Assembly Enables Low‐Threshold Lasing

Perovskite quantum dots (QDs) are of interest for solution‐processed lasers; however, their short Auger lifetime has limited lasing operation principally to the femtosecond temporal regime the photoexcitation levels to achieve optical gain threshold are up to two orders of magnitude higher in the na...

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Autores principales: Zhou, Chun, M. Pina, Joao, Zhu, Tong, H. Parmar, Darshan, Chang, Hao, Yu, Jie, Yuan, Fanglong, Bappi, Golam, Hou, Yi, Zheng, Xiaopeng, Abed, Jehad, Chen, Hao, Zhang, Jian, Gao, Yuan, Chen, Bin, Wang, Ya‐Kun, Chen, Haijie, Zhang, Tianju, Hoogland, Sjoerd, Saidaminov, Makhsud I., Sun, Liaoxin, Bakr, Osman M., Dong, Hongxing, Zhang, Long, H. Sargent, Edward
Formato: Online Artículo Texto
Lenguaje:English
Publicado: John Wiley and Sons Inc. 2021
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8529423/
https://www.ncbi.nlm.nih.gov/pubmed/34449133
http://dx.doi.org/10.1002/advs.202101125
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author Zhou, Chun
M. Pina, Joao
Zhu, Tong
H. Parmar, Darshan
Chang, Hao
Yu, Jie
Yuan, Fanglong
Bappi, Golam
Hou, Yi
Zheng, Xiaopeng
Abed, Jehad
Chen, Hao
Zhang, Jian
Gao, Yuan
Chen, Bin
Wang, Ya‐Kun
Chen, Haijie
Zhang, Tianju
Hoogland, Sjoerd
Saidaminov, Makhsud I.
Sun, Liaoxin
Bakr, Osman M.
Dong, Hongxing
Zhang, Long
H. Sargent, Edward
author_facet Zhou, Chun
M. Pina, Joao
Zhu, Tong
H. Parmar, Darshan
Chang, Hao
Yu, Jie
Yuan, Fanglong
Bappi, Golam
Hou, Yi
Zheng, Xiaopeng
Abed, Jehad
Chen, Hao
Zhang, Jian
Gao, Yuan
Chen, Bin
Wang, Ya‐Kun
Chen, Haijie
Zhang, Tianju
Hoogland, Sjoerd
Saidaminov, Makhsud I.
Sun, Liaoxin
Bakr, Osman M.
Dong, Hongxing
Zhang, Long
H. Sargent, Edward
author_sort Zhou, Chun
collection PubMed
description Perovskite quantum dots (QDs) are of interest for solution‐processed lasers; however, their short Auger lifetime has limited lasing operation principally to the femtosecond temporal regime the photoexcitation levels to achieve optical gain threshold are up to two orders of magnitude higher in the nanosecond regime than in the femtosecond. Here the authors report QD superlattices in which the gain medium facilitates excitonic delocalization to decrease Auger recombination and in which the macroscopic dimensions of the structures provide the optical feedback required for lasing. The authors develope a self‐assembly strategy that relies on sodiumd—an assembly director that passivates the surface of the QDs and induces self‐assembly to form ordered three‐dimensional cubic structures. A density functional theory model that accounts for the attraction forces between QDs allows to explain self‐assembly and superlattice formation. Compared to conventional organic‐ligand‐passivated QDs, sodium enables higher attractive forces, ultimately leading to the formation of micron‐length scale structures and the optical faceting required for feedback. Simultaneously, the decreased inter‐dot distance enabled by the new ligand enhances exciton delocalization among QDs, as demonstrated by the dynamically red‐shifted photoluminescence. These structures function as the lasing cavity and the gain medium, enabling nanosecond‐sustained lasing with a threshold of 25 µJ cm(–2).
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spelling pubmed-85294232021-10-27 Quantum Dot Self‐Assembly Enables Low‐Threshold Lasing Zhou, Chun M. Pina, Joao Zhu, Tong H. Parmar, Darshan Chang, Hao Yu, Jie Yuan, Fanglong Bappi, Golam Hou, Yi Zheng, Xiaopeng Abed, Jehad Chen, Hao Zhang, Jian Gao, Yuan Chen, Bin Wang, Ya‐Kun Chen, Haijie Zhang, Tianju Hoogland, Sjoerd Saidaminov, Makhsud I. Sun, Liaoxin Bakr, Osman M. Dong, Hongxing Zhang, Long H. Sargent, Edward Adv Sci (Weinh) Research Articles Perovskite quantum dots (QDs) are of interest for solution‐processed lasers; however, their short Auger lifetime has limited lasing operation principally to the femtosecond temporal regime the photoexcitation levels to achieve optical gain threshold are up to two orders of magnitude higher in the nanosecond regime than in the femtosecond. Here the authors report QD superlattices in which the gain medium facilitates excitonic delocalization to decrease Auger recombination and in which the macroscopic dimensions of the structures provide the optical feedback required for lasing. The authors develope a self‐assembly strategy that relies on sodiumd—an assembly director that passivates the surface of the QDs and induces self‐assembly to form ordered three‐dimensional cubic structures. A density functional theory model that accounts for the attraction forces between QDs allows to explain self‐assembly and superlattice formation. Compared to conventional organic‐ligand‐passivated QDs, sodium enables higher attractive forces, ultimately leading to the formation of micron‐length scale structures and the optical faceting required for feedback. Simultaneously, the decreased inter‐dot distance enabled by the new ligand enhances exciton delocalization among QDs, as demonstrated by the dynamically red‐shifted photoluminescence. These structures function as the lasing cavity and the gain medium, enabling nanosecond‐sustained lasing with a threshold of 25 µJ cm(–2). John Wiley and Sons Inc. 2021-08-27 /pmc/articles/PMC8529423/ /pubmed/34449133 http://dx.doi.org/10.1002/advs.202101125 Text en © 2021 The Authors. Advanced Science published by Wiley‐VCH GmbH https://creativecommons.org/licenses/by/4.0/This is an open access article under the terms of the http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.
spellingShingle Research Articles
Zhou, Chun
M. Pina, Joao
Zhu, Tong
H. Parmar, Darshan
Chang, Hao
Yu, Jie
Yuan, Fanglong
Bappi, Golam
Hou, Yi
Zheng, Xiaopeng
Abed, Jehad
Chen, Hao
Zhang, Jian
Gao, Yuan
Chen, Bin
Wang, Ya‐Kun
Chen, Haijie
Zhang, Tianju
Hoogland, Sjoerd
Saidaminov, Makhsud I.
Sun, Liaoxin
Bakr, Osman M.
Dong, Hongxing
Zhang, Long
H. Sargent, Edward
Quantum Dot Self‐Assembly Enables Low‐Threshold Lasing
title Quantum Dot Self‐Assembly Enables Low‐Threshold Lasing
title_full Quantum Dot Self‐Assembly Enables Low‐Threshold Lasing
title_fullStr Quantum Dot Self‐Assembly Enables Low‐Threshold Lasing
title_full_unstemmed Quantum Dot Self‐Assembly Enables Low‐Threshold Lasing
title_short Quantum Dot Self‐Assembly Enables Low‐Threshold Lasing
title_sort quantum dot self‐assembly enables low‐threshold lasing
topic Research Articles
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8529423/
https://www.ncbi.nlm.nih.gov/pubmed/34449133
http://dx.doi.org/10.1002/advs.202101125
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