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 NbOI2and 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.
Cui Yuanyuan,Wang Tingjun,Hu Deng,Wang Zhiwei,Hong Jiawang,Wang Xueyun
2-dimensional (2D) piezoelectric materials have gained significant attention due to their potential applications in flexible energy harvesting and storage devices. Recently, niobium oxide dihalides NbOI 2 stands out as a multifunctional anisotropic semiconductor family with an exceptionally high lateral piezoelectric constant (~21.8 pm/V), making it a promising candidate for energy conversion applications. Here we report the experimental observation of anisotropic in-plane piezoelectricity in multilayer NbOI 2 . Current-voltage relationships reveal a significant piezotronic effect in two typical crystalline orientations. Additionally, cyclic tensile and release experiments demonstrate an intrinsic current output of up to 140 pA when subjected to a tensile strain of 0.51%. A flexible piezoelectric nanogenerator prototype is demonstrated on the human finger and wrist, which opens up new avenues for the development of wearable electronic devices and provides valuable insights for further exploration in this field.
The spontaneous centrosymmetry-breaking and robust room-temperature ferroelectricity in niobium oxide dihalides spurs a flurry of explorations into its promising second-order nonlinear optical properties, and promises potential applications in nonvolatile electro-optical and optoelectronic devices. However, the ambient stability of the niobium oxide dihalides remains questionable, which overshadows their future development. In this work, the chemical degradation of NbOI2 is comprehensively investigated using combined chemical and optical microscopies in conjunction with spectroscopies. We unveil the highly anisotropic degradation kinetics of NbOI2 driven by the hydrolysis process of the unstable dangling iodine bonds dominantly on the (010) facet and progressing along the c axis. Knowing its degradation mechanism, the NbOI2 flake can then be stabilized by the hexagonal boron nitride encapsulation, which isolates the air moisture. These findings provide direct insights into the ambient instability of NbOI2, and they deliver possible solutions to circumvent this issue, which are essential for its practical integration in photonic and electronic devices.
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