Excitonic Bloch–Siegert shift in CsPbI3 perovskite quantum dots

Yuxuan Li, Yaoyao Han, Wenfei Liang, Boyu Zhang, Yulu Li, Yuan Liu, Yupeng Yang, Kaifeng Wu () and Jingyi Zhu ()
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Yuxuan Li: Chinese Academy of Sciences
Yaoyao Han: Chinese Academy of Sciences
Wenfei Liang: Chinese Academy of Sciences
Boyu Zhang: Chinese Academy of Sciences
Yulu Li: Chinese Academy of Sciences
Yuan Liu: Chinese Academy of Sciences
Yupeng Yang: Chinese Academy of Sciences
Kaifeng Wu: Chinese Academy of Sciences
Jingyi Zhu: Chinese Academy of Sciences

Nature Communications, 2022, vol. 13, issue 1, 1-8

Abstract: 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.

Date: 2022
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DOI: 10.1038/s41467-022-33314-9

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