Atomically Thin, Optically Isotropic Films with 3D Nanotopography

[Image: see text] Flat optics aims for the on-chip miniaturization of optical systems for high-speed and low-power operation, with integration of thin and lightweight components. Here, we present atomically thin yet optically isotropic films realized by using three-dimensional (3D) topographic reconstruction of anisotropic two-dimensional (2D) films to balance the out-of-plane and in-plane optical responses on the subwavelength scale. We achieve this by conformal growth of monolayer transition metal dichalcogenide (TMD) films on nanodome-structured substrates. The resulting films show an order-of-magnitude increase in the out-of-plane susceptibility for enhanced angular performance, displaying polarization isotropy in the off-axis absorption, as well as improved photoluminescence emission profiles, compared to their flat-film counterparts. We further show that such 3D geometric programming of optical properties is applicable to different TMD materials, offering spectral generalization over for the entire visible range. Our approach presents a powerful platform for advancing the development of atomically thin flat optics with custom-designed light–matter interactions.