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Charge carrier dynamics essentially determines the performance of various optoelectronic applications of colloidal semiconductor nanocrystals. Among them, two-dimensional nanoplatelets provide new adjustment freedom for their unique core/crown heterostructures. Herein, we demonstrate that by fine-tuning the core size and the lateral quantum confinement, the charge carrier transfer rate from the crown to the core can be varied by one order of magnitude in CdSe/CdSeS core/alloy-crown nanoplatelets. In addition, the transfer can be affected by a carrier blocking mechanism, i.e., the filled carriers hinder further possible transfer. Furthermore, we found that the biexciton interaction is oppositely affected by quantum confinement and electron delocalization, resulting in a non-monotonic variation of the biexciton binding energy with the emission wavelength. This work provides new observations and insights into the charge carrier transfer dynamics and exciton interactions in colloidal nanoplatelets and will promote their further applications in lasing, display, sensing, etc.


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Lateral quantum confinement regulates charge carrier transfer and biexciton interaction in CdSe/CdSeS core/crown nanoplatelets

Show Author's information Yige Yao1,§Xiaotian Bao2,§Yunke Zhu1Xinyu Sui2An Hu1Peng Bai1Shufeng Wang1,4,5,6Hong Yang1,4,5,6Xinfeng Liu2,3,7( )Yunan Gao1,4,5,6( )
State Key Laboratory for Artificial Microstructure and Mesoscopic Physics, School of Physics, Peking University, Beijing 100871, China
CAS Key Laboratory of Standardization and Measurement for Nanotechnology, National Center for Nanoscience and Technology, Beijing 100190, China
University of Chinese Academy of Sciences, Beijing 100049, China
Frontiers Science Center for Nano-optoelectronics, Beijing 100871, China
Collaborative Innovation Center of Extreme Optics, Shanxi University, Taiyuan 030006, China
Peking University Yangtze Delta Institute of Optoelectronics, Nantong 226010, China
Dalian National Laboratory for Clean Energy, Dalian 116023, China

§ Yige Yao and Xiaotian Bao contributed equally to this work.

Abstract

Charge carrier dynamics essentially determines the performance of various optoelectronic applications of colloidal semiconductor nanocrystals. Among them, two-dimensional nanoplatelets provide new adjustment freedom for their unique core/crown heterostructures. Herein, we demonstrate that by fine-tuning the core size and the lateral quantum confinement, the charge carrier transfer rate from the crown to the core can be varied by one order of magnitude in CdSe/CdSeS core/alloy-crown nanoplatelets. In addition, the transfer can be affected by a carrier blocking mechanism, i.e., the filled carriers hinder further possible transfer. Furthermore, we found that the biexciton interaction is oppositely affected by quantum confinement and electron delocalization, resulting in a non-monotonic variation of the biexciton binding energy with the emission wavelength. This work provides new observations and insights into the charge carrier transfer dynamics and exciton interactions in colloidal nanoplatelets and will promote their further applications in lasing, display, sensing, etc.

Keywords: ultrafast spectroscopy, biexciton, nanoplatelets, core/crown, charge carrier transfer

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Publication history
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Acknowledgements

Publication history

Received: 08 November 2022
Revised: 01 February 2023
Accepted: 03 February 2023
Published: 07 March 2023
Issue date: July 2023

Copyright

© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

This work was supported by the National Natural Science Foundation of China (No. 61875002), the National Key R&D Program of China (No. 2018YFA0306302), the Beijing Natural Science Foundation (No. Z190005), and the Program of State Key Laboratory of Quantum Optics and Quantum Optics Devices (No. KF202208). The author acknowledges the support of the Strategic Priority Research Program of Chinese Academy of Sciences (No. XDB36000000), and the National Natural Science Foundation of China (Nos. 11874130 and 22073022), and the support from the DNL Cooperation Fund, CAS (No. DNL202016) of Dalian National Laboratory for Clean Energy.

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