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arXiv · 2208.10045

Excitonic Bloch-Siegert shift in CsPbI3 perovskite quantum dots

Yuxuan Li·Yaoyao Han·Wenfei Liang·Boyu Zhang·Yulu Li·Yuan Liu·Yupeng Yang·Jingyi Zhu·Kaifeng Wu
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Abstract

Coherent interaction between matter and periodic light field induces both optical Stark effect (OSE) and Bloch-Siegert shift (BSS). Observing the BSS has been historically challenging, not only because it is weak but it is often accompanied by a much stronger OSE. Herein, by controlling the light helicity, we can largely restrict the OSE and BSS to different spin-transitions in CsPbI3 perovskite quantum dots, achieving room-temperature BSS as strong as 4 meV with near-infrared pulses. The ratio between the BSS and OSE magnitudes is however systematically higher than the prediction by the non-interacting, quasi-particle picture. With a model that explicitly accounts for excitonic effects, we quantitatively reproduce the experimental observations. This model depicts a unified physical picture of the interplay between the OSE, biexcitonic OSE and BSS 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.

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Yuxuan Li, Yaoyao Han, Wenfei Liang, Boyu Zhang, Yulu Li, Yuan Liu, Yupeng Yang, Jingyi Zhu, Kaifeng Wu. 2022-08-22. Excitonic Bloch-Siegert shift in CsPbI3 perovskite quantum dots. https://doi.org/10.1038/s41467-022-33314-9

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