Saturation of Two-Photon Absorption in Layered Transition Metal Dichalcogenides: Experiment and Theory

The saturation of two-photon absorption (TPA) in four types of layered transition metal dichalcogenides (TMDCs) (MoS₂, WS₂, MoSe₂, WSe₂) was systemically studied both experimentally and theoretically. It was demonstrated that the TPA coefficient is decreased when either the incident pulse intensity or the thickness of the TMDC nanofilms increases, while TPA saturation intensity has the opposite behavior, under the excitation of 1.2 eV photons with a pulse width of 350 fs. A three-level excitonic dynamics simulation indicates that the fast relaxation of the excitonic dark states, the exciton–exciton annihilation, and the depletion of electrons in the ground state contribute significantly to TPA saturation in TMDC nanofilms. Large third-order nonlinear optical responses make these layered 2D semiconductors strong candidate materials for optical modulation and other photonic applications

Dynamical Response of Nonlinear Optical Anisotropy in a Tin Sulfide Crystal under Ultrafast Photoexcitation

Analogous to black phosphorus, SnS processes folded structure that shows a strongly anisotropic optical absorption. Herein, by using ultrafast two-color pump and probe spectroscopy, the azimuthal angle dependence of nonlinear optical anisotropy in SnS is investigated. After 390 nm photoexcitation, the reflectivity of the 780 nm probe beam is first reduced significantly, followed by a complex alternation with the rotation of the sample along the c-axis. The relaxation of reflectivity consisted of two components: a 1–3 ps fast process that shows azimuthal angle and pump fluence dependence, which arises from electron–phonon coupling. The slow process shows strongly azimuthal angle dependence, which arises from the recovery of a photoinduced structural change, i.e., from the photoinduced metastable state with Cmcm-like symmetry to the initial state with Pnma symmetry. In addition, a coherent acoustic phonon with a frequency of 40 GHz is also identified, which originates from the temperature gradient-induced strain wave in the SnS crystal

Dynamical Response of Nonlinear Optical Anisotropy in a Tin Sulfide Crystal under Ultrafast Photoexcitation

Analogous to black phosphorus, SnS processes folded structure that shows a strongly anisotropic optical absorption. Herein, by using ultrafast two-color pump and probe spectroscopy, the azimuthal angle dependence of nonlinear optical anisotropy in SnS is investigated. After 390 nm photoexcitation, the reflectivity of the 780 nm probe beam is first reduced significantly, followed by a complex alternation with the rotation of the sample along the c-axis. The relaxation of reflectivity consisted of two components: a 1–3 ps fast process that shows azimuthal angle and pump fluence dependence, which arises from electron–phonon coupling. The slow process shows strongly azimuthal angle dependence, which arises from the recovery of a photoinduced structural change, i.e., from the photoinduced metastable state with Cmcm-like symmetry to the initial state with Pnma symmetry. In addition, a coherent acoustic phonon with a frequency of 40 GHz is also identified, which originates from the temperature gradient-induced strain wave in the SnS crystal

Direct Observation of Degenerate Two-Photon Absorption and Its Saturation in WS₂ and MoS₂ Monolayer and Few-Layer Films

The optical nonlinearity of WS₂ and MoS₂ monolayer and few-layer films was investigated using the <i>Z</i>-scan technique with femtosecond pulses from the visible to the near-infrared range. The nonlinear absorption of few- and multilayer WS₂ and MoS₂ films and their dependences on excitation wavelength were studied. WS₂ films with 1–3 layers exhibited a giant two-photon absorption (TPA) coefficient as high as (1.0 ± 0.8) × 10⁴ cm/GW. TPA saturation was observed for the WS₂ film with 1–3 layers and for the MoS₂ film with 25–27 layers. The giant nonlinearity of WS₂ and MoS₂ films is attributed to a two-dimensional confinement, a giant exciton effect, and the band edge resonance of TPA