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Discovering new types of layered perovskites has great importance for designing novel optoelectronic devices. In this article, combining first‐principle calculations with global structure searching, it is found that Rb4SnSb2Br12, a typical halide double perovskite, can unexpectedly possess fertile low formation‐energy polymorphs holding van de Walls (vdW) layered structures. Consequently, these polymorphs...
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