Irreversible coherent matching bonding of van der Waals heterostructure lattice by pressure.

The key of heterostructure is the combinations created by stacking various vdW materials, which can modify interlayer coupling and electronic properties, providing exciting opportunities for designer devices. However, this simple stacking does not create chemical bonds, making it difficult to fundamentally alter the electronic structure. Here, we demonstrate that interlayer interactions in heterostructures can be fundamentally controlled using hydrostatic pressure, providing a bonding method to modify electronic structures. By covering graphene with boron nitride and inducing an irreversible phase transition, the conditions for graphene lattice-matching bonding (IMB) were created. We demonstrate that the increased bandgap of graphene under pressure is well maintained in ambient due to the IMB in the interface. Comparison to theoretical modeling emphasizes the process of pressure-induced interfacial bonding, systematically generalizes, and predicts this model. Our results demonstrate that pressure can irreversibly control interlayer bonding, providing opportunities for high-pressure technology in ambient applications and IMB engineering in heterostructures.