Mechanism of Extreme Optical Nonlinearities in Spiral WS2 above the Bandgap

Layered two-dimensional transition-metal dichalcogenides (2D-TMDs) are promising building blocks for ultracompact optoelectronic applications. Recently, a strong second harmonic generation (SHG) was observed in spiral stacked TMD nanostructures which was explained by its low crystal symmetry. However, the relationship between the efficiency of SHG signals and the electronic band structure remains unclear. Here, we show that the SHG signal in spiral WS2 nanostructures is strongly enhanced (similar to 100 fold increase) not only when the second harmonic signal is in resonance with the exciton states but also when the excitation energy is slightly above the electronic band gap, which we attribute to a large interband Berry connection associated with certain optical transitions in spiral WS2. The giant SHG enhancement observed and explained in this study could promote the understanding and utility of TMDs as highly efficient nonlinear optical materials and potentially lead to a new pathway to fabricate more efficient optical energy conversion devices.