Enhanced third-harmonic generation by manipulating the twist angle of bilayer graphene

Twisted bilayer graphene (tBLG) has received substantial attention in various research fields due to its unconventional physical properties originating from Moiré superlattices. The electronic band structure in tBLG modified by interlayer interactions enables the emergence of low-energy van Hove singularities in the density of states, allowing the observation of intriguing features such as increased optical conductivity and photocurrent at visible or near-infrared wavelengths. Here, we show that the third-order optical nonlinearity can be considerably modified depending on the stacking angle in tBLG. The third-harmonic generation (THG) efficiency is found to significantly increase when the energy gap at the van Hove singularity matches the three-photon resonance of incident light. Further study on electrically tuneable optical nonlinearity reveals that the gate-controlled THG enhancement varies with the twist angle in tBLG, resulting in a THG enhanced up to 60 times compared to neutral monolayer graphene. Our results prove that the twist angle opens up a new way to control and increase the optical nonlinearity of tBLG, suggesting rotation-induced tuneable nonlinear optics in stacked two-dimensional material systems. Nonlinear optics: When graphene ‘does the twist’ Modifying the angle between the two layers of twisted bilayer graphene can considerably improve how photons interact with it to generate higher-energy photons. Dong-Il Yeom of Ajou University and colleagues in Korea shined laser light onto twisted bilayer graphene stacked at various angles, and measured the outcoming optical signals. Twisted bilayer graphene is made by stacking two monolayer graphenes at an angle. The interlayer interaction in this material leads to intriguing properties. The scientists found that changing the angle could enhance a nonlinear optical property, called third-harmonic generation, by 60 times compared to monolayer graphene. The team then conducted Raman measurements and modeling calculations to understand how this process occurs. They say their findings could pave the way towards novel designs for enhancing optical nonlinearity in two-dimensional stacked materials.