Structural stability, electronic structure, and magnetism of the $d^9$ double infinite-layer La${}_3$Ni${}_2$O${}_5$F under chemical pressure and epitaxial strain

Abstract

Nickelate materials exhibit rich electronic properties that can be engineered toward cuprate-like regimes through topotactic and mixed-anion chemistry. Using first-principles calculations, we investigate the newly synthesized double infinite-layer oxyfluoride La${}_3$Ni${}_2$O${}_5$F and its evolution under chemical pressure and epitaxial strain. The calculated phonon spectrum confirms the dynamical stability of the reported double infinite-layer crystal structure. Further, we find a highly two-dimensional cuprate-like Fermi surface dominated by Ni-$d_{x^2-y^2}$ states, with a moderate rare-earth-derived self-doping yielding an effective $\sim d_{x^2-y^2}^{1.2}$ filling. These electronic features remain remarkably robust under both chemical pressure and epitaxial strain. Spin-polarized calculations further reveal an extended manifold of nearly degenerate magnetic configurations with different in-plane and out-of-plane spin arrangements. Compressive strain further enhances this magnetic frustration while leaving the underlying electronic structure largely unchanged. Our results thus identify La${}_3$Ni${}_2$O${}_5$F as a promising cuprate analogue and establish lattice engineering as an effective strategy for fine tuning its electronic and magnetic properties.

8 + 3 pages, 6 + 7 figs