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Nano-engineered electron–hole exchange interaction controls exciton dynamics in core–shell semiconductor nanocrystals

Author

Listed:
  • S. Brovelli

    (Los Alamos National Laboratory)

  • R.D. Schaller

    (Los Alamos National Laboratory
    Center for Advanced Solar Photophysics, Los Alamos National Laboratory)

  • S.A. Crooker

    (National High Magnetic Field Laboratory, Los Alamos National Laboratory)

  • F. García-Santamaría

    (Los Alamos National Laboratory)

  • Y. Chen

    (Los Alamos National Laboratory)

  • R. Viswanatha

    (Los Alamos National Laboratory)

  • J.A. Hollingsworth

    (Los Alamos National Laboratory
    Center for Integrated Nanotechnologies, Los Alamos National Laboratory)

  • H. Htoon

    (Los Alamos National Laboratory
    Center for Advanced Solar Photophysics, Los Alamos National Laboratory
    Center for Integrated Nanotechnologies, Los Alamos National Laboratory)

  • V.I. Klimov

    (Los Alamos National Laboratory
    Center for Advanced Solar Photophysics, Los Alamos National Laboratory)

Abstract

A strong electron–hole exchange interaction (EI) in semiconductor nanocrystals (NCs) gives rise to a large (up to tens of meV) splitting between optically active ('bright') and optically passive ('dark') excitons. This dark–bright splitting has a significant effect on the optical properties of band-edge excitons and leads to a pronounced temperature and magnetic field dependence of radiative decay. Here we demonstrate a nanoengineering-based approach that provides control over EI while maintaining nearly constant emission energy. We show that the dark–bright splitting can be widely tuned by controlling the electron–hole spatial overlap in core–shell CdSe/CdS NCs with a variable shell width. In thick-shell samples, the EI energy reduces to

Suggested Citation

  • S. Brovelli & R.D. Schaller & S.A. Crooker & F. García-Santamaría & Y. Chen & R. Viswanatha & J.A. Hollingsworth & H. Htoon & V.I. Klimov, 2011. "Nano-engineered electron–hole exchange interaction controls exciton dynamics in core–shell semiconductor nanocrystals," Nature Communications, Nature, vol. 2(1), pages 1-8, September.
    • Handle: RePEc:nat:natcom:v:2:y:2011:i:1:d:10.1038_ncomms1281
    DOI: 10.1038/ncomms1281
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    Cited by:

    1. Zhen Han & Chunbo Duan & Xi-Yan Dong & Yubing Si & Jia-Hua Hu & Yan Wang & Si-Meng Zhai & Tian Lu & Hui Xu & Shuang-Quan Zang, 2025. "Tightly bonded excitons in chiral metal clusters for luminescent brilliance," Nature Communications, Nature, vol. 16(1), pages 1-12, December.

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