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Dimensionality-induced insulator-metal crossover in layered nickelates La n+1
= 2, 3, and ∞)
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Low-valence layered nickelates are a structural analog to the superconducting cuprates and possess interesting properties. In this work, we have systematically studied the electronic structure of La n+1 Ni n O2n+2 using first-principles calculations. Our results reveal that the Ni-3d 3z 2 − r 2 orbital state is active and evolves from discrete molecular levels to a continuous solid band and its filling varies as the dimensionality (or n) increases. The two-dimensional (2D) La3 Ni 2O6 and La4 Ni 3O8 are thus found to have a molecular insulating state. In contrast, the 3D LaNiO2 is metallic and its 3z 2 − r 2 band surprisingly becomes 3D due to the Ni-La hybridization, and the La-5d xy orbital also forms a 2D metallic band. Therefore, La n+1 Ni n O2n+2 is a dimensionality-controlled insulator-metal crossover system.
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