Electronic structure trends in La$_{2}R$Ni$_2$O$_7$ ($R=$ Pr, Nd, Sm) from first-principles

Abstract

The discovery of superconductivity in bilayer La$_3$Ni$_2$O$_7$ under pressure has sparked tremendous attention on Ruddlesden-Popper (RP) nickelates. Recently, a higher superconducting transition temperature of 96 K was reported in Sm-doped La$_3$Ni$_2$O$_7$ single crystals at $\sim$ 22 GPa. Motivated by this experimental observation, we systematically explore the crystal structure and electronic properties of La$_3$Ni$_2$O$_7$ doped with different rare-earth elements in comparison to the undoped counterpart. As expected due to the effect of chemical pressure, we find that the volume of La$_{2}$$R$Ni$_2$O$_7$ ($R=$ Pr, Nd, Sm) progressively decreases with doping from Pr to Sm. We further find a pressure-induced structural transition to tetragonal symmetry that approximately coincides with the emergence of superconductivity in all cases. This transition is characterized by the emergence of flat $d_{z^2}$ bands at the Fermi level in the electronic structure. Despite subtle distinctions in the electronic structure between undoped and $R$-doped La$_3$Ni$_2$O$_7$, an increase in the dominant planar hopping is obtained as the $R$ size decreases. In contrast, the out-of-plane hopping decreases (in spite of the $c$ lattice constant compression), due to the decrease in the apical Ni-O$_{\rm rocksalt}$ bond length. Our findings provide further microscopic insights into the effects of $R$-doping in the electronic structure of RP nickelate superconductors in connection to $T_c$.