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Heteroepitaxy with large lattice mismatch remains a great challenge for high‐quality epifilm growth. Although great efforts have been devoted to epifilm growth with an in‐plane lattice mismatch, the epitaxy of 2D layered crystals on stepped substrates with a giant out‐of‐plane lattice mismatch is seldom reported. Here, taking the molecular‐beam epitaxy of 2D semiconducting Bi2O2Se on 3D SrTiO3 substrates...
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