2D layered nanomaterials as photocatalysts have attracted much attention in the field of solar hydrogen production due to their unique electronic structure and abundant active sites. Nevertheless, the rational design and interfacial regulation of 2D Z‐scheme heterojunction are still challenging. Herein, an ultrathin 2D ZnIn2S4/g‐C3N4 Z‐scheme heterojunction is precisely constructed via in‐situ growth of ZnIn2S4 on the g‐C3N4. By carefully regulating the interface structure in heterojunction, the hydrogen evolution performance can be greatly improved. The optimized photocatalyst exhibits a remarkable photocatalytic activity without Pt as cocatalyst, which is primarily ascribed to the synergistic effect of abundant active sites, enhanced photoresponse, and valid interfacial charge transfer channels. Meanwhile, the spectroscopic analyses and density functional theory (DFT) calculation results comprehensively prove that the promoted interfacial charge separation in 2D Z‐scheme heterojunction is another key factor for the enhanced photocatalytic performance. This work offers a new avenue for the rational design of ultrathin Z‐scheme heterojunction photocatalysts with improved photocatalytic performance through interfacial engineering.

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Multifunctional polarization controlling plays an important role in modern photonics, but their designs toward broad bandwidths and high efficiencies are still rather challenging. Here, by applying the inverse design method of model-based theoretical paradigm, we design cascaded chiral metamaterials for different polarization controls in oppositely propagating directions and demonstrate their broadband and high-efficiency performance theoretically and experimentally. Started with the derivation of scattering matrix towards specified polarization control, a chiral metamaterial is designed as a meta-quarter-wave plate for the forward propagating linearly polarized wave, which converts the x-or y-polarized wave into a nearly perfect left-or right-handed circularly polarized wave; intriguingly, it also serves as a 45°polarization rotator for the backward propagating linearly polarized waves. This bifunctional metamaterial shows a high transmission as well as a broad bandwidth due to the Fabry-Perot-like interference effect. Using the similar approach, an abnormal broadband meta-quarter-wave plate is achieved to convert the forward x-and y-polarized or the backward y-and x-polarized waves into left-and right-handed circularly polarized waves with high transmission efficiencies. The integration of multiple functions in a single structure endows the cascaded chiral metamaterials with great interests for the high-efficiency polarization-controlled applications.npj Computational Materials (2019) 5:93; https://doi.