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Colloidal, Room-Temperature Growth of Metal Oxide Shells on InP Quantum Dots

  • Nayon Park
    Nayon Park
    Department of Chemistry, University of Washington, Seattle, Washington 98195, United States
    More by Nayon Park
  • Ryan A. Beck
    Ryan A. Beck
    Department of Chemistry, University of Washington, Seattle, Washington 98195, United States
    More by Ryan A. Beck
  • Kevin K. Hoang
    Kevin K. Hoang
    Department of Chemistry, University of Washington, Seattle, Washington 98195, United States
  • Dylan M. Ladd
    Dylan M. Ladd
    Department of Materials Science and Engineering, University of Colorado, Boulder, Colorado 80309, United States
  • Jared E. Abramson
    Jared E. Abramson
    Department of Physics, University of Washington, Seattle, Washington 98195, United States
  • Ricardo A. Rivera-Maldonado
    Ricardo A. Rivera-Maldonado
    Department of Chemistry, University of Washington, Seattle, Washington 98195, United States
  • Hao A. Nguyen
    Hao A. Nguyen
    Department of Chemistry, University of Washington, Seattle, Washington 98195, United States
  • Madison Monahan
    Madison Monahan
    Department of Chemistry, University of Washington, Seattle, Washington 98195, United States
  • Gerald T. Seidler
    Gerald T. Seidler
    Department of Physics, University of Washington, Seattle, Washington 98195, United States
  • Michael F. Toney
    Michael F. Toney
    Department of Materials Science and Engineering, Chemical and Biological Engineering, Renewable and Sustainable Energy Institute, University of Colorado, Boulder, Colorado 80309, United States
  • Xiaosong Li
    Xiaosong Li
    Department of Chemistry, University of Washington, Seattle, Washington 98195, United States
    More by Xiaosong Li
  • , and 
  • Brandi M. Cossairt*
    Brandi M. Cossairt
    Department of Chemistry, University of Washington, Seattle, Washington 98195, United States
    *Email: [email protected]
Cite this: Inorg. Chem. 2023, 62, 17, 6674–6687
Publication Date (Web):April 12, 2023
https://doi.org/10.1021/acs.inorgchem.3c00161
Copyright © 2023 American Chemical Society

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    Abstract

    Abstract Image

    We demonstrate colloidal, layer-by-layer growth of metal oxide shells on InP quantum dots (QDs) at room temperature. We show with computational modeling that native InP QD surface oxides give rise to nonradiative pathways due to the presence of surface-localized dark states near the band edges. Replacing surface indium with zinc to form a ZnO shell results in reduced nonradiative decay and a density of states at the valence band edge that resembles defect-free, stoichiometric InP. We then developed a synthetic strategy using stoichiometric amounts of common atomic layer deposition precursors in alternating cycles to achieve layer-by-layer growth. Metal-oxide-shelled InP QDs show bulk and local structural perturbations as determined by X-ray diffraction and extended X-ray absorption fine structure spectroscopy. Upon growing ZnSe shells of varying thickness on the oxide-shelled QDs, we observe increased photoluminescence (PL) quantum yields and narrowing of the emission linewidths that we attribute to decreased ion diffusion to the shell, as supported by phosphorus X-ray emission spectroscopy. These results present a versatile strategy to control QD interfaces for novel heterostructure design by leveraging surface oxides. This work also contributes to our understanding of the connections between structural complexity and PL properties in technologically relevant colloidal optoelectronic materials.

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.inorgchem.3c00161.

    • Additional experimental details, DFT models and calculation details, and supporting characterization (PDF)

    • In77P77H108.xyz (XYZ)

    • In77P31O46H108.xyz (XYZ)

    • In31P31Al46O46H108.xyz (XYZ)

    • In31P31Cd46O46H108.xyz (XYZ)

    • In31P31Ga46O46H108.xyz (XYZ)

    • In31P31Zn46O46H108.xyz (XYZ)

    • In31P77Al46H108.xyz (XYZ)

    • In31P77Cd46H108.xyz (XYZ)

    • In31P77Ga46H108.xyz (XYZ)

    • In31P77Zn46H108.xyz (XYZ)

    • In31P31H50.xyz (XYZ)

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    Cited By

    This article is cited by 2 publications.

    1. Philippe B. Green, Ona Segura Lecina, Petru P. Albertini, Mark A. Newton, Krishna Kumar, Coline Boulanger, Jari Leemans, Paul B.J. Thompson, Anna Loiudice, Raffaella Buonsanti. Colloidal Atomic Layer Deposition on Nanocrystals Using Ligand-Modified Precursors. Journal of the American Chemical Society 2024, 146 (15) , 10708-10715. https://doi.org/10.1021/jacs.4c00538
    2. Xian Wei, Qi Zhang, Zhongjie Cui, Dan Yang, Shiliang Mei, Wanlu Zhang, Haijiao Xie, Kehan Yu, Ruiqian Guo, Wei Wei. Mapping the Identity of Transition Metal Doping and Surface Passivation in Indium Phosphide with Theoretical Calculation. Inorganic Chemistry 2023, 62 (37) , 15258-15266. https://doi.org/10.1021/acs.inorgchem.3c02455

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