期刊
NANO LETTERS
卷 20, 期 5, 页码 3003-3018出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.9b04870
关键词
nanocrystals; nanoplatelets; c-ALD; PASS-PIETA; dynamic nuclear polarization; solid-state NMR
类别
资金
- European Union through the FP7 (ERC Starting Grant NANOSOLID) [GA 306733]
- European Union through Horizon 2020 research and innovation program (ERC project SCALE-HALO) [819740]
- ERC Advanced Grant [320860]
- Scholarship Fond of the Swiss Chemical Industry (SSCI Award 2015)
- Scholarship Fond of the Swiss Chemical Industry (SSCI Award 2017)
- European Research Council (ERC) [320860] Funding Source: European Research Council (ERC)
Ligand exchange and CdS shell growth onto colloidal CdSe nanoplatelets (NPLs) using colloidal atomic layer deposition (c-ALD) were investigated by solid-state nuclear magnetic resonance (NMR) experiments, in particular, dynamic nuclear polarization (DNP) enhanced phase adjusted spinning sidebands-phase incremented echo-train acquisition (PASS-PIETA). The improved sensitivity and resolution of DNP enhanced PASS-PIETA permits the identification and study of the core, shell, and surface species of CdSe and CdSe/CdS core/shell NPLs heterostructures at all stages of c-ALD. The cadmium chemical shielding was found to be proportionally dependent on the number and nature of coordinating chalcogen-based ligands. DFT calculations permitted the separation of the the Cd-111/113 chemical shielding into its different components, revealing that the varying strength of paramagnetic and spin-orbit shielding contributions are responsible for the chemical shielding trend of cadmium chalcogenides. Overall, this study points to the roughening and increased chemical disorder at the surface during the shell growth process, which is not readily captured by the conventional characterization tools such as electron microscopy.
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