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3D ZrSe5 crystals are layered compounds with very weak interlayer bonding, from which a stable 2D system can easily be obtained. Using density functional theory (DFT), it is predicted that bulk ZrSe5 is a weak topological insulator (WTI) with a bandgap of 0.157 eV and that single‐layer ZrSe5 is a promising candidate for quantum spin Hall (QSH) insulators, with a direct bandgap as large as 0.183 eV...
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