Pressure and strain tuning of the alternating bilayer-trilayer Ruddlesden-Popper nickelate: crystal and electronic structure

Abstract

We use first-principles calculations to investigate the crystal and electronic structure of the hybrid bilayer-trilayer Ruddlesden-Popper (RP) nickelate La$_7$Ni$_5$O$_{17}$ under hydrostatic pressure and biaxial compressive strain. By analyzing the irreducible representations of the dynamically unstable phonon modes in the high-symmetry $P4/mmm$ structure, we identify a dynamically stable lower-symmetry $C2/c$ structure containing octahedral tilts. The application of both pressure and compressive strain tends to suppress the octahedral tilts, effectively tetragonalizing the structure, in analogy with the conventional RPs. The electronic structure under hydrostatic pressure and strain has similarities, but it differs in the position of the $d_{z^2}$ bonding band from the trilayer block. This band crosses the Fermi level at a pressure of 30 GPa, but it remains below it for any level of compressive strain. This strain-induced modification mirrors the electronic structure changes observed in the conventional bilayer nickelate.