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Heteroepitaxial chemistry of zinc chalcogenides on InP nanocrystals for defect-free interfaces with atomic uniformity

Author

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  • Yeongho Choi

    (Sungkyunkwan University (SKKU)
    Sungkyunkwan University)

  • Donghyo Hahm

    (Sungkyunkwan University, Suwon
    Los Alamos National Laboratory)

  • Wan Ki Bae

    (Sungkyunkwan University, Suwon)

  • Jaehoon Lim

    (Sungkyunkwan University (SKKU)
    Sungkyunkwan University)

Abstract

Heteroepitaxy on colloidal semiconductor nanocrystals is an essential strategy for manipulating their optoelectronic functionalities. However, their practical synthesis typically leads to scattered and unexpected outcomes due to the intervention of multiple reaction pathways associated with complicated side products of reactants. Here, the heteroepitaxy mechanism of zinc chalcogenide initiated on indium phosphide (InP) colloidal nanocrystals is elucidated using the precursors, zinc carboxylate and trialkylphosphine selenide. The high magnetic receptivity of 77Se and the characteristic longitudinal optical phonon mode of ZnSe allowed for monitoring the sequence of epilayer formation at the molecular level. The investigation revealed the sterically hindered acyloxytrialkylphosphonium and diacyloxytrialkylphosphorane to be main intermediates in the surface reaction, which retards the metal ion adsorption by a large steric hindrance. The transformation of adsorbates to the crystalline epilayer was disturbed by surface oxides. Raman scattering disclosed the pathway of secondary surface oxidation triggered by carboxylate ligands migrated from zinc carboxylate. The surface-initiated heteroepitaxy protocol is proposed to fabricate core/shell heterostructured nanocrystals with atomic-scale uniformity of epilayers. Despite the large lattice mismatch of ZnS to InP, we realised a uniform and interface defect-free ZnS epilayer (~0.3 nm thickness) on InP nanocrystals, as evidenced by a high photoluminescence quantum yield of 97.3%.

Suggested Citation

  • Yeongho Choi & Donghyo Hahm & Wan Ki Bae & Jaehoon Lim, 2023. "Heteroepitaxial chemistry of zinc chalcogenides on InP nanocrystals for defect-free interfaces with atomic uniformity," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-022-35731-2
    DOI: 10.1038/s41467-022-35731-2
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    References listed on IDEAS

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    1. Jung Hoon Song & Hyekyoung Choi & Hien Thu Pham & Sohee Jeong, 2018. "Energy level tuned indium arsenide colloidal quantum dot films for efficient photovoltaics," Nature Communications, Nature, vol. 9(1), pages 1-9, December.
    2. Victor I. Klimov & Sergei A. Ivanov & Jagjit Nanda & Marc Achermann & Ilya Bezel & John A. McGuire & Andrei Piryatinski, 2007. "Single-exciton optical gain in semiconductor nanocrystals," Nature, Nature, vol. 447(7143), pages 441-446, May.
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