The collective response of macroscopic quantum states under perturbation is widely used to study quantum correlations and cooperative properties, such as defect-induced quantum vortices in Bose–Einstein condensates and the non-destructive scattering of impurities in superfluids. Superfluorescence (SF), as a collective effect rooted in dipole–dipole cooperation through virtual photon exchange, leads to the macroscopic dipole moment (MDM) in high-density dipole ensembles. However, the perturbation response of the MDM in SF systems remains unknown. Echo-like behavior is observed in a cooperative exciton ensemble under a controllable perturbation, corresponding to an initial collapse followed by a revival of the MDM. Such a dynamic response could refer to a phase transition between the macroscopic coherence regime and the incoherent classical state on a time scale of 10 ps. The echo-like behavior is absent above 100 K due to the instability of MDM in a strongly dephased exciton ensemble. Experimentally, the MDM response to perturbations is shown to be controlled by the amplitude and injection time of the perturbations.

This work reports the real-time observation of the interlayer lattice vibrations in bilayer and few-layer PtSe2 by means of the coherent phonon method. The layer-breathing mode and standing wave mode of the interlayer vibrations are found to coexist in such a kind of group-10 transition metal dichalcogenides (TMDCs). The interlayer breathing force constant standing for perpendicular coupling (per effective atom) is derived as 7.5 N/m, 2.5 times larger than that of graphene. The interlayer shearing force constant is comparable to the interlayer breathing force constant, which indicates that PtSe2 has nearly isotropic interlayer coupling. The low-frequency Raman spectroscopy elucidates the polarization behavior of the layer-breathing mode that is assigned to have A1g symmetry. The standing wave mode shows redshift with the increasing number of layers, which successfully determines the out-of-plane sound velocity of PtSe2 experimentally. Our results manifest that the coherent phonon method is a good tool to uncover the interlayer lattice vibrations, beyond the conventional Raman spectroscopy limit. The strong interlayer interaction in group-10 TMDCs reveals their promising potential in high-frequency (～terahertz) micro-mechanical resonators.

Mechanical exfoliation (ME) and chemical vapor deposition (CVD) MoS₂ monolayers have been extensively studied, but the large differences of nonlinear optical performance between them have never been clarified. Here, we prepared MoS₂ monolayers using ME and CVD methods and investigated the two-photon absorption (TPA) response and its saturation. We found that the TPA coefficient of the ME monolayer was about (1.88 ± 0.21) × 10³ cm/GW, nearly two times that of the CVD one at (1.04 ± 0.15) × 10³ cm/GW. Furthermore, we simulated and compared the TPA-induced optical pulse modulation in multilayer cascaded structures, which is instructive and meaningful for the design of optical devices such as a beam shaper and optical limiter.

Questions hovering over the modulation of bandgap size and excitonic effect on nonlinear absorption in two-dimensional transition metal dichalcogenides (TMDCs) have restricted their application in micro/nano optical modulator, optical switching, and beam shaping devices. Here, degenerate two-photon absorption (TPA) in the near-infrared region was studied experimentally in mechanically exfoliated MoS2 from single layer to multilayer. The layer-dependent TPA coefficients were significantly modulated by the detuning of the excitonic dark state (2p). The shift of the quasiparticle bandgap and the decreasing of exciton binding energy with layers were deduced, combined with the non-hydrogen model of excitons in TMDCs and the scaling rule of semiconductors. Our work clearly demonstrates the layer modulation of nonlinear absorption in TMDCs and provides support for layer-dependent nonlinear optical devices, such as optical limiters and optical switches.

This work presents the saturable absorption (SA) properties of CsPbBr3 perovskite quantum dots (QDs). The perovskite QDs show excellent SA performance with a nonlinear absorption coefficient of ?35×10?2 cm/GW and a figure of merit of 3.7×10?14 esu?cm. Further, their use as saturable absorbers in a passively Q-switched visible solid-state laser for the generation of soliton pulses is demonstrated. These results demonstrate the potential for the perovskite QDs to act as saturable absorbers.