Excitonic Bloch-Siegert shift in CsPbI3 perovskite quantum dots
arXiv:2208.10045 · doi:10.1038/s41467-022-33314-9
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.
References in corpus (6)
- Observation of the Bloch-Siegert Shift in a Qubit-Oscillator System in the Ultrastrong Coupling Regime
- Ultrafast Generation of Pseudo-magnetic Field for Valley Excitons in WSe2 Monolayers
- The impact of the halide cage on the electronic properties of fully inorganic caesium lead halide perovskites
- Large, valley-exclusive Bloch-Siegert shift in monolayer WS2
- Lattice distortion inducing exciton splitting and coherent quantum beating in CsPbI3 perovskite quantum dots
- Observation of intervalley biexcitonic optical Stark effect in monolayer WS2