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

Go Yumoto, Hideki Hirori, Fumiya Sekiguchi, Ryota Sato, Masaki Saruyama, Toshiharu Teranishi and Yoshihiko Kanemitsu ()
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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

Nature Communications, 2021, vol. 12, issue 1, 1-7

Abstract: 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.

Date: 2021
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DOI: 10.1038/s41467-021-23291-w

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