Abstract
Perovskite nickelates RNiO(3) (R = rare-earth ion) exhibit complex rare-earth ion dependent phase diagram and high tunability of various appealing properties. Here, combining first- and finite-temperature second-principles calculations, we explicitly demonstrate that the superior merits of the interplay among lattice, electron, and spin degrees of freedom can be passed to RNiO(2), which recently gained significant interest as superconductors. We unveil that decreasing the rare-earth size directly modulates the structural, electronic, and magnetic properties and naturally groups infinite-layer nickelates into two categories in terms of the Fermi surface and magnetic dimensionality: compounds with large rare-earth sizes (La, Pr) closely resemble the key properties of CaCuO(2), showing quasi-two-dimensional (2D) antiferromagnetic (AFM) correlations and strongly localized dx2-y2 orbitals around the Fermi level; the compounds with small rare-earth sizes (Nd-Lu) are highly analogous to ferropnictides, showing three-dimensional (3D) magnetic dimensionality and strong kz dispersion of d3z2-r2 electrons at the Fermi level. Additionally, we highlight that RNiO(2) with R = Nd-Lu exhibit on cooling a structural transition with the appearance of oxygen rotation motion, which is softened by the reduction of rare-earth size and enhanced by spin-rotation couplings. The rare-earth control of kz dispersion and structural phase transition might be the key factors differentiating the distinct upper critical field and resistivity in different compounds. The established original phase diagram summarizing the temperature and rare-earth controlled structural, electronic, and magnetic transitions in RNiO(2) compounds provides rich structural and chemical flexibility to tailor the superconducting property.