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Colloidal-ALD-Grown Core/Shell CdSe/CdS Nanoplatelets as Seen by DNP Enhanced PASS-PIETA NMR Spectroscopy.

Laura Piveteau1,2, Dmitry N Dirin1,2, Christopher P Gordon1

  • 1Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir Prelog Weg 1-5, Zurich CH-8093, Switzerland.

Nano Letters
|February 21, 2020
PubMed
Summary
This summary is machine-generated.

This study used advanced NMR techniques to analyze cadmium selenide/cadmium sulfide (CdSe/CdS) core/shell nanoplatelets during shell growth. Results reveal surface disorder not visible with electron microscopy.

Keywords:
PASS−PIETAc-ALDdynamic nuclear polarizationnanocrystalsnanoplateletssolid-state NMR

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Area of Science:

  • Materials Science
  • Nanotechnology
  • Solid-State Chemistry

Background:

  • Colloidal atomic layer deposition (c-ALD) is crucial for synthesizing core/shell nanoplatelets (NPLs).
  • Understanding surface chemistry during shell growth is vital for controlling NPL properties.
  • Conventional characterization methods like electron microscopy have limitations in probing surface disorder.

Purpose of the Study:

  • To investigate ligand exchange and CdS shell growth on CdSe NPLs using c-ALD.
  • To characterize the core, shell, and surface species of CdSe/CdS heterostructures at various c-ALD stages.
  • To elucidate the factors influencing cadmium chemical shielding in these nanostructures.

Main Methods:

  • Solid-state nuclear magnetic resonance (NMR) experiments, specifically dynamic nuclear polarization (DNP) enhanced phase adjusted spinning sidebands-phase incremented echo-train acquisition (PASS-PIETA).
  • Density Functional Theory (DFT) calculations to analyze 111/113Cd chemical shielding components.
  • Characterization of CdSe and CdSe/CdS core/shell NPLs throughout the c-ALD process.

Main Results:

  • DNP-enhanced PASS-PIETA provided high sensitivity and resolution for studying NPLs.
  • Cadmium chemical shielding correlated with the type and number of coordinating chalcogen-based ligands.
  • DFT analysis revealed paramagnetic and spin-orbit shielding contributions dictate the chemical shielding trend.
  • Evidence of surface roughening and increased chemical disorder during CdS shell growth was observed.

Conclusions:

  • Advanced NMR techniques offer unique insights into nanoparticle surface chemistry during synthesis.
  • Surface disorder during shell growth is a significant factor affecting NPL properties.
  • The findings highlight limitations of conventional characterization tools for detailed surface analysis.