▎ 摘　　要

van der Waals heterostructures formed by stacking various atomically thin crystals have been proved to be a powerful approach to explore designer materials with nearly limitless new properties. Here, we report nonperturbative high harmonic generation (HHG) in two-dimensional (2D) heterostructures combining graphene and hexagonal boron nitride (G/hBN). First-principles calculation results reveal that the G/hBN bilayer extends the HHG properties of the constituent layers. Harmonic intensity can be significantly enhanced by several orders of magnitude by tuning the Berry curvature of G/hBN via pressure-controlled interlayer interaction. The result offers a new way to enhance HHG in graphene. It also demonstrates that van der Waals heterostructures and their novel degrees of freedom can be used to control the HHG process and open up more possibilities to manipulate strong-field ultrafast physical properties in such 2D materials.