Xiaoyue Fan

The niobium oxide dihalides have recently been identified as a new class of van der Waals materials exhibiting exceptionally large second-order nonlinear optical responses and robust in-plane ferroelectricity. In contrast to second-order nonlinear processes, third-order optical nonlinearities can arise irrespective of whether a crystal lattice is centrosymmetric. Here, we report third harmonic generation (THG) in two-dimensional (2D) transition metal oxide iodides, namely NbOI₂ and TaOI₂. We observe a comparable THG intensity from both materials. By benchmarking against THG from monolayer WS₂, we deduce that the third-order susceptibility is approximately on the same order. THG resonances are revealed at different excitation wavelengths, likely due to enhancement by excitonic states and band edge resonances. The THG intensity increases for material thicknesses up to 30 nm, owing to weak interlayer coupling. After this threshold, it shows saturation or a decrease, due to optical interference effects. Our results establish niobium and tantalum oxide iodides as promising 2D materials for third-order nonlinear optics, with intrinsic in-plane ferroelectricity and thickness-tunable nonlinear efficiency.

In 2H stacking bilayer MoS₂, the exciton with an interlayer nature has been evidenced due to the hybridization of hole states among both layers. The transition energy of this interlayer exciton is located between the A and B excitons. In this work, we investigate the evolution of optical properties in stacking MoS₂ bilayers with the twisted angles ranging from 0° to 60°, especially focusing on the interlayer exciton. The clear modulations of the exciton responses are observed by the room-temperature reflectance. The interlayer exciton transition is observed in the artificial stacking bilayer MoS₂ with the twisted angle around 60°. We found that the interlayer exciton is very sensitive to the twisted angle. Once the stacking angle deviates the 2H stacking by a few degrees, the interlayer transition is quenched. This is due to the bilayer symmetry and interlayer coupling of this unique system.

Controlling the interlayer coupling by tuning lattice parameters through pressure engineering is an important route for tailoring the optoelectronic properties of two-dimensional materials. In this work, we report a pressure-dependent study on the exciton transitions of bilayer MoS₂ exfoliated on a diamond anvil surface. The applied hydrostatic pressure changes from ambient pressure up to 11.05 GPa using a diamond anvil cell device. Raman, photoluminescence, and reflectivity spectra at room temperature are analyzed to characterize the interlayer coupling of this bilayer system. With the increase of pressure, the indirect exciton emission disappears completely at about 5 GPa. Importantly, we clearly observed the interlayer exciton from the reflectivity spectra, which becomes invisible at a low pressure around 1.26 GPa. This indicates that the interlayer exciton is very sensitive to the hydrostatic pressure due to the oscillator strength transfer from the direct transition to the indirect one.