Publication date: 8th June 2021
Colloidal quantum dots (cQDs) have found important applications in fields spanning from medicine to electronic and optoelectronic devices. However, their stability under ambient and processing conditions remains an unsolved challenge. The growth of inert and stable metal-oxide shells can overcome this issue. Our group has recently developed a colloidal atomic layer deposition (c-ALD) approach which provides a methodology capable to grow such oxide shells with tunable thickness around different cores. [1]
In this work, we use NMR spectroscopy to obtain deeper mechanistic insights into the key role played by the ligands during the nucleation and growth stages. CdSe@AlOx cQDs are selected as the model system because of the extensive knowledge on the surface chemistry of the pristine CdSe cQDs. First of all, titration experiments in solution 1H-NMR indicate that the original oleate ligands contribute to the nucleation of the alumina shell. Solid-state NMR 13C-27Al correlation experiments with dynamic nuclear polarization (DNP) enhancement corroborate this ligand-driven nucleation mechanism of the organometallic precursors on the QD surface. Thanks to this newly acquired knowledge, we demonstrate that tuning the ligand density is a tool to control the cross-linking degree of the shell, thus opening up different opportunities for these new core@shell structures.
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