期刊
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 11, 期 9, 页码 3339-3344出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.0c00870
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资金
- SIM-Flanders (SBOQDOCCO)
- FWO-Vlaanderen [17006602]
- Ghent University [01G01019]
- FWO-vlaanderen
- FWO [FWO17/PDO/184]
- European Research Counsil [815128, 714876]
- SURF Cooperative
- European Research Council (ERC) [714876] Funding Source: European Research Council (ERC)
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.
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