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Strong spin-orbit coupling inducing Autler-Townes effect in lead halide perovskite nanocrystals

Author

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  • Go Yumoto

    (Institute for Chemical Research, Kyoto University)

  • Hideki Hirori

    (Institute for Chemical Research, Kyoto University)

  • Fumiya Sekiguchi

    (Institute for Chemical Research, Kyoto University)

  • Ryota Sato

    (Institute for Chemical Research, Kyoto University)

  • Masaki Saruyama

    (Institute for Chemical Research, Kyoto University)

  • Toshiharu Teranishi

    (Institute for Chemical Research, Kyoto University)

  • Yoshihiko Kanemitsu

    (Institute for Chemical Research, Kyoto University)

Abstract

Manipulation of excitons via coherent light-matter interaction is a promising approach for quantum state engineering and ultrafast optical modulation. Various excitation pathways in the excitonic multilevel systems provide controllability more efficient than that in the two-level system. However, these control schemes have been restricted to limited control-light wavelengths and cryogenic temperatures. Here, we report that lead halide perovskites can lift these restrictions owing to their multiband structure induced by strong spin-orbit coupling. Using CsPbBr3 perovskite nanocrystals, we observe an anomalous enhancement of the exciton energy shift at room temperature with increasing control-light wavelength from the visible to near-infrared region. The enhancement occurs because the interconduction band transitions between spin-orbit split states have large dipole moments and induce a crossover from the two-level optical Stark effect to the three-level Autler-Townes effect. Our finding establishes a basis for efficient coherent optical manipulation of excitons utilizing energy states with large spin-orbit splitting.

Suggested Citation

  • Go Yumoto & Hideki Hirori & Fumiya Sekiguchi & Ryota Sato & Masaki Saruyama & Toshiharu Teranishi & Yoshihiko Kanemitsu, 2021. "Strong spin-orbit coupling inducing Autler-Townes effect in lead halide perovskite nanocrystals," Nature Communications, Nature, vol. 12(1), pages 1-7, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-23291-w
    DOI: 10.1038/s41467-021-23291-w
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    Cited by:

    1. 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.

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