Abstract Recently, while investigating the crystal-plane- and crystal-orientation-dependent properties of materials, we discovered that a polar superstructure featuring a spontaneous electric field (Es) governs these very physical and chemical behaviors. In this Spotlight article, we discuss the enhanced properties of such polar superstructures and propose a universal model that elucid the underlying mechanisms in photocatalysis, the bulk photovoltaic effect, gas sensing, the piezoelectric effect, thermovoltaics, and chem-voltaics. Consequently, a broadly influential field of polar superstructure electronics and optoelectronics is established, where the underlying physics is based on the control of electrons and photogenerated electrons by the Es within polar superstructures. This theory not only reinterprets fundamental material properties but also unlocks atomic-scale routes for the rational design and fabrication of high-performance materials and devices. Polar superstructure materials are poised to become a major frontier in materials, chemistry, and physics.
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