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To enable new nonlinear responses, metamaterials are created by organizingstructural units (meta-atoms) which are typically on the scale of about ahundred nanometers. However, truly altering atomic symmetry and enabling newnonlinear responses requires control at the atomic-scale, down to a fewangstroms. Here we report the discovery of 3D nonlinear optical metamaterialsrealized by the precise control and twist of individual 2D van der Waalsinterfaces. Specifically, new nonlinear crystals are achieved by adding pseudoscrew symmetries to a multiple of 4-layer WS2 stacks (e.g. 4-layer, 8-layer,etc). The nonlinear susceptibility of the resulting 3D crystal is fundamentallydifferent from natural WS2. Furthermore, we show that the magnitude of thenewly enabled nonlinearity is enhanced by controlling the number of interfacesand the excitation wavelength. Our findings suggest a new approach toredesigning intrinsic nonlinearity in artificial atomic configurations,scalable from a few nanometer-thick unit cells to bulk materials.

3D nonlinear optical metamaterials from twisted 2D van der Waals interfaces