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Single-exciton optical gain in semiconductor nanocrystals

Author

Listed:
  • Victor I. Klimov

    (Los Alamos National Laboratory, Los Alamos, New Mexico 87545, USA)

  • Sergei A. Ivanov

    (Los Alamos National Laboratory, Los Alamos, New Mexico 87545, USA)

  • Jagjit Nanda

    (Los Alamos National Laboratory, Los Alamos, New Mexico 87545, USA)

  • Marc Achermann

    (Los Alamos National Laboratory, Los Alamos, New Mexico 87545, USA)

  • Ilya Bezel

    (Los Alamos National Laboratory, Los Alamos, New Mexico 87545, USA)

  • John A. McGuire

    (Los Alamos National Laboratory, Los Alamos, New Mexico 87545, USA)

  • Andrei Piryatinski

    (Los Alamos National Laboratory, Los Alamos, New Mexico 87545, USA)

Abstract

Nanocrystal quantum dots have favourable light-emitting properties. They show photoluminescence with high quantum yields, and their emission colours depend on the nanocrystal size—owing to the quantum-confinement effect—and are therefore tunable. However, nanocrystals are difficult to use in optical amplification and lasing. Because of an almost exact balance between absorption and stimulated emission in nanoparticles excited with single electron–hole pairs (excitons), optical gain can only occur in nanocrystals that contain at least two excitons. A complication associated with this multiexcitonic nature of light amplification is fast optical-gain decay induced by non-radiative Auger recombination, a process in which one exciton recombines by transferring its energy to another. Here we demonstrate a practical approach for obtaining optical gain in the single-exciton regime that eliminates the problem of Auger decay. Specifically, we develop core/shell hetero-nanocrystals engineered in such a way as to spatially separate electrons and holes between the core and the shell (type-II heterostructures). The resulting imbalance between negative and positive charges produces a strong local electric field, which induces a giant (∼100 meV or greater) transient Stark shift of the absorption spectrum with respect to the luminescence line of singly excited nanocrystals. This effect breaks the exact balance between absorption and stimulated emission, and allows us to demonstrate optical amplification due to single excitons.

Suggested Citation

  • 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.
  • Handle: RePEc:nat:nature:v:447:y:2007:i:7143:d:10.1038_nature05839
    DOI: 10.1038/nature05839
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    Cited by:

    1. Hanlin Fang & Qiaoling Lin & Yi Zhang & Joshua Thompson & Sanshui Xiao & Zhipei Sun & Ermin Malic & Saroj P. Dash & Witlef Wieczorek, 2023. "Localization and interaction of interlayer excitons in MoSe2/WSe2 heterobilayers," Nature Communications, Nature, vol. 14(1), pages 1-7, December.
    2. Yuxuan Li & Yaoyao Han & Wenfei Liang & Boyu Zhang & Yulu Li & Yuan Liu & Yupeng Yang & Kaifeng Wu & Jingyi Zhu, 2022. "Excitonic Bloch–Siegert shift in CsPbI3 perovskite quantum dots," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    3. 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.
    4. Philippe Tamarat & Elise Prin & Yuliia Berezovska & Anastasiia Moskalenko & Thi Phuc Tan Nguyen & Chenghui Xia & Lei Hou & Jean-Baptiste Trebbia & Marios Zacharias & Laurent Pedesseau & Claudine Katan, 2023. "Universal scaling laws for charge-carrier interactions with quantum confinement in lead-halide perovskites," Nature Communications, Nature, vol. 14(1), pages 1-8, December.
    5. Heeyoung Jung & Young-Shin Park & Namyoung Ahn & Jaehoon Lim & Igor Fedin & Clément Livache & Victor I. Klimov, 2022. "Two-band optical gain and ultrabright electroluminescence from colloidal quantum dots at 1000 A cm−2," Nature Communications, Nature, vol. 13(1), pages 1-8, December.

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