Excitonic Bloch–Siegert shift in CsPbI3 perovskite quantum dots

Li, Yuxuan; Han, Yaoyao; Zhang, Boyu; Li, Yulu; Liu, Yuan; Yang, Yupeng; Wu, Kaifeng; Zhu, Jingyi

doi:10.1038/s41467-022-33314-9

Cited by 12 publications

(3 citation statements)

References 55 publications

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“…Earlier experiments offer at least two possibilities: the Bloch-Siegert effect or a contribution from the quantum confined Stark effect. The Bloch-Siegert effect has been found in perovskite nanocrystals [32] and transition metal dichalcogenides [33]. However, although the Bloch-Siegert effect becomes relatively more prominent with larger detuning, this is not considered the likely origin as Bloch-Siegert effects are typically concurrent with OSE unless spin selectivity is specifically controlled-which it is not in this dataand the signals are weaker and similar spectrally to OSE.…”

Section: Resultsmentioning

confidence: 57%

Optical stark effect on CdSe nanoplatelets with mid-infrared excitation for large amplitude ultrafast modulation

Diroll¹

2023

Nanotechnology

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The optical Stark effect is a universal response of the electronic structure to incident light. In semiconductors, particularly nanomaterials, the optical Stark effect achieved with sub-band gap photons can drive large, narrowband, and potentially ultrafast changes in the absorption or reflection at the band gap through excitation of virtual excitons. Rapid optical modulation using the optical Stark effect is ultimately constrained, however, by the generation of long-lived excitons through multiphoton absorption. This work compares the modulation achievable using the optical Stark effect on CdSe nanoplatelets with several different pump photon energies, from the visible to mid-infrared. Despite expected lower efficiencies for spectrally-remote pump energies, infrared pump pulses can ultimately drive larger sub-picosecond optical Stark shifts of virtual excitons without creation of real excitons. The CdSe nanoplatelets show subpicosecond shifts of the lowest excitonic resonance of up to 22 meV, resulting in change in absorption as large as 0.32 OD (49 % increase in transmission), with a long-lived offset from real excitons less than 1 % of the peak signal.

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Section: Resultsmentioning

confidence: 57%

Optical stark effect on CdSe nanoplatelets with mid-infrared excitation for large amplitude ultrafast modulation

Diroll¹

2023

Nanotechnology

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“…In σ + σ + configuration, the blueshift excitonic band is evident and explained perfectly by the optical-Stark effect, but in σ + σconfiguration, the blueshifted band is rare. The latter one can be realized at very high detuning e.g., infrared excitation for such a system (Eg = ~2.09 eV), and is known as the Bloch-Siegert effect [8]. In previously reported observation, at low detuning or nearly resonant excitation, the shift in σ + σ + excitation is explained by considering rotating wave approximation and dropping the fast-rotating terms.…”

Section: Resultsmentioning

confidence: 94%

Anomalous excitonic shift under near-resonant excitation in Cu-doped CsPbI3

Sharma,

Bose,

Ray

et al. 2024

Nonlinear Optics and Its Applications 2024

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The interaction of nonresonant intense periodic optical field shifts the ground state excitonic position which can be understood by Floquet manipulation in Jaynes-Cummings model. The induced shift can be manifested by the optical Stark effect (OSE) and Bloch-Siegert effect (BSE) via controlling the light helicity. It is noteworthy that the energy shift is proportional to field intensity and inversely to the detuning at nearly resonant excitation which understood by rotating wave approximation. Recently, OSE and BSE have observed simultaneously with very large detuning (infrared excitation) for CsPbI3 quantum dots. However, observing the BSE at near resonance with small detuning is difficult due to the dominance shift by OSE. Here, we have chosen Cu-doped CsPbI3 nanocrystals and incorporated a helicity-resolved transient absorption spectroscopic technique. Moreover, the dynamical excitonic effect in a small percentage of Cu-doping reduced the binding energy and blueshifted the continuum band without changing the excitonic position. Interestingly we observe blueshift in excitonic position for co (σ + σ + )-and cross(σ + σ -)-polarization of pump and probe at small detuning. We observed a huge BSE shift ~ 122 meV with the ratios of shifts (i.e., ΔBSE/ΔOSE) are 0.74 at the lowest detuning, 193 meV Cu-doped CsPbI3, respectively. Thus, our study advances high-field Floquet engineering with a doping mechanism and can be potentially exploited in strong-field device applications as well as a quantum information process.

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“…Photon-dressed states, also known as Floquet states, can emerge in a few-level system periodically driven by strong optical fields. The hybridization between these dressed states and the bare states leads to the formation of novel quantum states. − Such coherent light–matter interactions enable optical control of electronic states in atoms, , quantum dots, , GaAs quantum wells, − and atomically thin transition metal dichalcogenides (TMDs). − These effects, such as the optical Stark effect (OSE), ,, Autler–Townes splitting, ,, and the Bloch–Siegert shift, ,− can serve as prerequisites for optical operation in quantum information science. In the past few years, spin-selective OSE has been demonstrated in both bulk and two-dimensional (2D) layered perovskites. , These materials offer the advantage of facile solution processability and scalability, making them highly promising for applications in ultrafast photonics and spintronics.…”

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confidence: 99%

Floquet Engineering of Excitons in Two-Dimensional Halide Perovskites via Biexciton States

Cai,

Feng,

Kanwat

et al. 2024

Nano Lett.

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Layered two-dimensional halide perovskites (2DHPs) exhibit exciting non-equilibrium properties that allow the manipulation of energy levels through coherent light−matter interactions. Under the Floquet picture, novel quantum states manifest through the optical Stark effect (OSE) following intense subresonant photoexcitation. Nevertheless, a detailed understanding of the influence of strong many-body interactions between excitons on the OSE in 2DHPs remains unclear. Herein, we uncover the crucial role of biexcitons in photon-dressed states and demonstrate precise optical control of the excitonic states via the biexcitonic OSE in 2DHPs. With fine step tuning of the driven energy, we fully parametrize the evolution of exciton resonance modulation. The biexcitonic OSE enables Floquet engineering of the exciton resonance with either a blue-shift or a red-shift of the energy levels. Our findings shed new light on the intricate nature of coherent light−matter interactions in 2DHPs and extend the degree of freedom for ultrafast coherent optical control over excitonic states.

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Excitonic Bloch–Siegert shift in CsPbI3 perovskite quantum dots

Cited by 12 publications

References 55 publications

Optical stark effect on CdSe nanoplatelets with mid-infrared excitation for large amplitude ultrafast modulation

Optical stark effect on CdSe nanoplatelets with mid-infrared excitation for large amplitude ultrafast modulation

Anomalous excitonic shift under near-resonant excitation in Cu-doped CsPbI3

Floquet Engineering of Excitons in Two-Dimensional Halide Perovskites via Biexciton States

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