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Hot-Carrier Relaxation in CdSe/CdS Core/Shell Nanoplatelets
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    Hot-Carrier Relaxation in CdSe/CdS Core/Shell Nanoplatelets
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    • Matthew Pelton*
      Matthew Pelton
      Department of Physics, UMBC (University of Maryland, Baltimore County), Baltimore, Maryland 21250, United States
      Center for Nanoscale Materials, Argonne National Laboratory, Argonne, Illinois 60439, United States
      *E-mail: [email protected]
    • Yana Wang
      Yana Wang
      School of Engineering, The University of British Columbia, Kelowna, British Columbia V1V 1V7, Canada
      More by Yana Wang
    • Igor Fedin
      Igor Fedin
      Department of Chemistry and James Franck Institute, University of Chicago, Chicago, Illinois 60637, United States
      More by Igor Fedin
    • Dmitri V. Talapin
      Dmitri V. Talapin
      Center for Nanoscale Materials, Argonne National Laboratory, Argonne, Illinois 60439, United States
      Department of Chemistry and James Franck Institute, University of Chicago, Chicago, Illinois 60637, United States
    • Stephen K. O’Leary
      Stephen K. O’Leary
      School of Engineering, The University of British Columbia, Kelowna, British Columbia V1V 1V7, Canada
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    The Journal of Physical Chemistry C

    Cite this: J. Phys. Chem. C 2020, 124, 1, 1020–1026
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    https://doi.org/10.1021/acs.jpcc.9b08006
    Published December 11, 2019
    Copyright © 2019 American Chemical Society

    Abstract

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    We present time-resolved photoluminescence (PL) spectroscopy of a series of colloidal CdSe/CdS core/shell nanoplatelets with different core and shell thicknesses. Exciton numbers are determined from the integrated PL intensities, and carrier temperatures are determined from the high-energy exponential tail of the PL spectra. For times between 10 and 1000 ps, the measured carrier relaxation dynamics are well described by a simple model of Auger reheating: biexcitonic Auger recombination continually increases the average energy of the carriers (while decreasing their number), and this reheating sets a bottleneck to cooling through electron–phonon coupling. For times between 1 and 10 ps, the relaxation dynamics are consistent with electron–phonon coupling, where the bottleneck is now the decay of the longitudinal optical phonon population. Comparison of relaxation dynamics to recombination dynamics reveals changes in the carrier–phonon coupling for shell thicknesses greater than 4 monolayers.

    Copyright © 2019 American Chemical Society

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    Cited By

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    This article is cited by 11 publications.

    1. Benjamin T. Diroll, Corentin Dabard, Muchuan Hua, Juan I. Climente, Emmanuel Lhuillier, Sandrine Ithurria. Hole Relaxation Bottlenecks in CdSe/CdTe/CdSe Lateral Heterostructures Lead to Bicolor Emission. Nano Letters 2024, 24 (26) , 7934-7940. https://doi.org/10.1021/acs.nanolett.4c01250
    2. Sunil Gyawali, Ravi Teja A. Tirumala, Harrison Loh, Marimuthu Andiappan, Alan D. Bristow. Photocarrier Recombination Dynamics in Highly Scattering Cu2O Nanocatalyst Clusters. The Journal of Physical Chemistry C 2024, 128 (5) , 2003-2011. https://doi.org/10.1021/acs.jpcc.3c06941
    3. Benjamin T. Diroll, Burak Guzelturk, Hong Po, Corentin Dabard, Ningyuan Fu, Lina Makke, Emmanuel Lhuillier, Sandrine Ithurria. 2D II–VI Semiconductor Nanoplatelets: From Material Synthesis to Optoelectronic Integration. Chemical Reviews 2023, 123 (7) , 3543-3624. https://doi.org/10.1021/acs.chemrev.2c00436
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    5. Junling Qu, Prachi Rastogi, Charlie Gréboval, Clément Livache, Marion Dufour, Audrey Chu, Sang-Soo Chee, Julien Ramade, Xiang Zhen Xu, Sandrine Ithurria, Emmanuel Lhuillier. Nanoplatelet-Based Light-Emitting Diode and Its Use in All-Nanocrystal LiFi-like Communication. ACS Applied Materials & Interfaces 2020, 12 (19) , 22058-22065. https://doi.org/10.1021/acsami.0c05264
    6. Yi Zhang, Rui Wang, Hongyu Yang, Jiayu Zhang, Gavin Conibeer. Review of carrier thermalization mechanisms in II-VI QDs and their potential application as the absorber in hot carrier solar cells. Solar Energy Materials and Solar Cells 2024, 272 , 112923. https://doi.org/10.1016/j.solmat.2024.112923
    7. Yi Zhang, Wenbin Xiang, Rui Wang, Jiayu Zhang, Gavin Conibeer. Study of the mechanisms of the phonon bottleneck effect in CdSe/CdS core/shell quantum dots and nanoplatelets and their application in hot carrier multi-junction solar cells. Nanoscale Advances 2023, 5 (20) , 5594-5600. https://doi.org/10.1039/D3NA00557G
    8. Laszlo Frazer, Jiho Han, Nicholas Kirkwood, Alison M. Funston. Blinking of CdSe/Cd .33 Zn .67 S semiconductor nanoplatelets. Journal of the Optical Society of America B 2023, 40 (6) , 1550. https://doi.org/10.1364/JOSAB.487184
    9. Yong Pan, Li Wang, Yan Zhang, Xueqiong Su, Dongwen Gao, Ruixiang Chen, Lun Huang, Wei Sun, Yuxin Zhao, Dangli Gao. Multi‐Wavelength Laser Emission by Hot‐Carriers Transfers in Perovskite‐Graphene‐Chalcogenide Quantum Dots. Advanced Optical Materials 2022, 10 (21) https://doi.org/10.1002/adom.202201044
    10. Ilia A. Vovk, Vladimir V. Lobanov, Aleksandr P. Litvin, Mikhail Yu. Leonov, Anatoly V. Fedorov, Ivan D. Rukhlenko. Band Structure and Intersubband Transitions of Three-Layer Semiconductor Nanoplatelets. Nanomaterials 2020, 10 (5) , 933. https://doi.org/10.3390/nano10050933
    11. Matthew Pelton. Colloidal Quantum Wells for High-Efficiency Lasers. 2020, JTh3G.3. https://doi.org/10.1364/NOMA.2020.JTh3G.3

    The Journal of Physical Chemistry C

    Cite this: J. Phys. Chem. C 2020, 124, 1, 1020–1026
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jpcc.9b08006
    Published December 11, 2019
    Copyright © 2019 American Chemical Society

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