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Near-edge ligand stripping and robust radiative exciton recombination in CdSe/CdS core/crown nanoplatelets

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Abstract
We address the relation between surface chemistry and optoelectronic properties in semiconductor nanocrystals using core/crown CdSe/CdS nanoplatelets passivated by cadmium oleate (Cd(Ol)(2)) as model systems. We show that addition of butylamine to a nanoplatelet (NPL) dispersion maximally displaces similar to 40% of the original Cd(Ol)(2) capping. On the basis of density functional theory simulations, we argue that this behavior reflects the preferential displacement of Cd(Ol)(2) from (near)-edge surface sites. Opposite from CdSe core NPLs, core/crown NPL dispersions can retain 45% of their initial photoluminescence efficiency after ligand displacement, while radiative exciton recombination keeps dominating the luminescent decay. Using electron microscopy observations, we assign this robust photoluminescence to NPLs with a complete CdS crown, which prevents charge carrier trapping in the near-edge surface sites created by ligand displacement. We conclude that Z-type ligands such as cadmium carboxylates can provide full electronic passivation of (100) facets yet are prone to displacement from near-edge surface sites.
Keywords
General Materials Science, QUANTUM DOTS, NANOCRYSTALS, DISPLACEMENT, SPECTROSCOPY, PROSPECTS

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MLA
Leemans, Jari, et al. “Near-Edge Ligand Stripping and Robust Radiative Exciton Recombination in CdSe/CdS Core/Crown Nanoplatelets.” JOURNAL OF PHYSICAL CHEMISTRY LETTERS, vol. 11, no. 9, 2020, pp. 3339–44, doi:10.1021/acs.jpclett.0c00870.
APA
Leemans, J., Singh, S., Li, C., Ten Brinck, S., Bals, S., Infante, I., … Hens, Z. (2020). Near-edge ligand stripping and robust radiative exciton recombination in CdSe/CdS core/crown nanoplatelets. JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 11(9), 3339–3344. https://doi.org/10.1021/acs.jpclett.0c00870
Chicago author-date
Leemans, Jari, Shalini Singh, Chen Li, Stephanie Ten Brinck, Sara Bals, Ivan Infante, Iwan Moreels, and Zeger Hens. 2020. “Near-Edge Ligand Stripping and Robust Radiative Exciton Recombination in CdSe/CdS Core/Crown Nanoplatelets.” JOURNAL OF PHYSICAL CHEMISTRY LETTERS 11 (9): 3339–44. https://doi.org/10.1021/acs.jpclett.0c00870.
Chicago author-date (all authors)
Leemans, Jari, Shalini Singh, Chen Li, Stephanie Ten Brinck, Sara Bals, Ivan Infante, Iwan Moreels, and Zeger Hens. 2020. “Near-Edge Ligand Stripping and Robust Radiative Exciton Recombination in CdSe/CdS Core/Crown Nanoplatelets.” JOURNAL OF PHYSICAL CHEMISTRY LETTERS 11 (9): 3339–3344. doi:10.1021/acs.jpclett.0c00870.
Vancouver
1.
Leemans J, Singh S, Li C, Ten Brinck S, Bals S, Infante I, et al. Near-edge ligand stripping and robust radiative exciton recombination in CdSe/CdS core/crown nanoplatelets. JOURNAL OF PHYSICAL CHEMISTRY LETTERS. 2020;11(9):3339–44.
IEEE
[1]
J. Leemans et al., “Near-edge ligand stripping and robust radiative exciton recombination in CdSe/CdS core/crown nanoplatelets,” JOURNAL OF PHYSICAL CHEMISTRY LETTERS, vol. 11, no. 9, pp. 3339–3344, 2020.
@article{8661804,
  abstract     = {We address the relation between surface chemistry and optoelectronic properties in semiconductor nanocrystals using core/crown CdSe/CdS nanoplatelets passivated by cadmium oleate (Cd(Ol)(2)) as model systems. We show that addition of butylamine to a nanoplatelet (NPL) dispersion maximally displaces similar to 40% of the original Cd(Ol)(2) capping. On the basis of density functional theory simulations, we argue that this behavior reflects the preferential displacement of Cd(Ol)(2) from (near)-edge surface sites. Opposite from CdSe core NPLs, core/crown NPL dispersions can retain 45% of their initial photoluminescence efficiency after ligand displacement, while radiative exciton recombination keeps dominating the luminescent decay. Using electron microscopy observations, we assign this robust photoluminescence to NPLs with a complete CdS crown, which prevents charge carrier trapping in the near-edge surface sites created by ligand displacement. We conclude that Z-type ligands such as cadmium carboxylates can provide full electronic passivation of (100) facets yet are prone to displacement from near-edge surface sites.},
  author       = {Leemans, Jari and Singh, Shalini and Li, Chen and Ten Brinck, Stephanie and Bals, Sara and Infante, Ivan and Moreels, Iwan and Hens, Zeger},
  issn         = {1948-7185},
  journal      = {JOURNAL OF PHYSICAL CHEMISTRY LETTERS},
  keywords     = {General Materials Science,QUANTUM DOTS,NANOCRYSTALS,DISPLACEMENT,SPECTROSCOPY,PROSPECTS},
  language     = {eng},
  number       = {9},
  pages        = {3339--3344},
  title        = {Near-edge ligand stripping and robust radiative exciton recombination in CdSe/CdS core/crown nanoplatelets},
  url          = {http://dx.doi.org/10.1021/acs.jpclett.0c00870},
  volume       = {11},
  year         = {2020},
}

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