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Quantification of a PbClx Shell on the Surface of PbS Nanocrystals

Author(s)
Winslow, Samuel W.; Liu, Yun; Swan, James W; Tisdale, William
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Abstract
Differences between the properties of PbS nanocrystals prepared using a large excess of PbCl2 and those prepared using other Pb sources have led to speculation that a thin PbClx shell may be present on the surface of PbCl2-derived PbS nanocrystals. However, characterization of this chloride layer has proven to be challenging because of the poor contrast provided by electron and X-ray scattering probes. Here, we show that small-angle neutron scattering (SANS) provides the compositional sensitivity needed to unambiguously quantify the PbClx shell that is present on the surface of PbCl2-derived PbS nanocrystals. Using a charge-balanced structural model, the scattering contribution of a ∼0.3 nm thick surface PbClx layer is parsed separately from ligand carboxylate head groups and PbS in the core. Global fitting of the SANS data across a solvent deuteration series enables unique determination of the spatial distribution of each material. These results are corroborated by quantitative nuclear magnetic resonance (NMR) and energy-dispersive X-ray spectroscopy (EDS). This work resolves a discrepancy in reported sizing curves for PbS nanocrystals prepared by different syntheses and further demonstrates the power of SANS in resolving molecular structure in soft and hybrid nanomaterials. Keyword: Quantum dots; Ligands; Layers; Solvents Nanocrystals
Date issued
2019-06
URI
https://hdl.handle.net/1721.1/123840
Department
Massachusetts Institute of Technology. Department of Chemical Engineering
Journal
ACS Materials Lettters
Publisher
American Chemical Society (ACS)
Citation
Winslow, Samuel W. et al. "Quantification of a PbClx Shell on the Surface of PbS Nanocrystals." ACS Materials Letters 1, 2, (June 2019): 209-216 © 2019 American Chemical Society
Version: Final published version
ISSN
2639-4979
2639-4979

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