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We performed ab initio calculations for the PbTiO3/SrTiO3 (001) heterostructures. For both PbO and TiO2‐terminations of the PbTiO3 (001) thin film, augmented on the SrTiO3 (001) substrate, the magnitudes of atomic relaxations Δz increases as a function of the number of augmented monolayers. For both terminations of the augmented PbTiO3 (001) nanothin film, all upper, third and fifth monolayers are...
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