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Excitonic Bloch–Siegert shift in CsPbI3 perovskite quantum dots

Author

Listed:
  • Yuxuan Li

    (Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

  • Yaoyao Han

    (Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

  • Wenfei Liang

    (Chinese Academy of Sciences)

  • Boyu Zhang

    (Chinese Academy of Sciences
    Hubei University of Art and Science)

  • Yulu Li

    (Chinese Academy of Sciences)

  • Yuan Liu

    (Chinese Academy of Sciences
    University of Science and Technology of China)

  • Yupeng Yang

    (Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

  • Kaifeng Wu

    (Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

  • Jingyi Zhu

    (Chinese Academy of Sciences)

Abstract

Coherent interaction between matter and light field induces both optical Stark effect and Bloch–Siegert shift. Observing the latter has been historically challenging, because it is weak and is often accompanied by a much stronger Stark shift. Herein, by controlling the light helicity, we can largely restrict these two effects to different spin-transitions in CsPbI3 perovskite quantum dots, achieving room-temperature Bloch–Siegert shift as strong as 4 meV with near-infrared pulses. The ratio between the Bloch–Siegert and optical Stark shifts is however systematically higher than the prediction by the non-interacting, quasi-particle model. With a model that explicitly accounts for excitonic effects, we quantitatively reproduce the experimental observations. This model depicts a unified physical picture of the optical Stark effect, biexcitonic optical Stark effect and Bloch–Siegert shift in low-dimensional materials displaying strong many-body interactions, forming the basis for the implementation of these effects to information processing, optical modulation and Floquet engineering.

Suggested Citation

  • 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.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-33314-9
    DOI: 10.1038/s41467-022-33314-9
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