Evolution of correlated electronic states of La2NiO4 under hydrostatic pressure

Abstract

We elucidate the electronic structure and quantum many-body instabilities of the monolayer nickelate La2NiO4 under hydrostatic pressure using a combination of density functional theory, dynamical mean-field theory (DFT+DMFT), and random phase approximation (RPA). Our DFT+DMFT calculations reveal non-Fermi-liquid behavior and coherence loss near the Fermi level at low pressures, driven by strong electron correlations within the Ni-e_g orbital manifold, which is analogous to the low-energy electronic properties observed in La3Ni2O7. However, multi-orbital spin susceptibility analysis demonstrates an exceptionally suppressed critical Stoner parameter U_c (about 0.4~0.7 eV), indicating robust magnetic order that dominates the ground state and precludes superconductivity in the pristine system. Below U_c, superconducting instabilities exhibit a pressure-driven symmetry transition: the d_(x2-y2)-wave pairing prevails at ambient and low pressure, while the s+g-wave symmetry occurs above 75 GPa. This transition is attributed to pressure-induced self-doping effect. The high-angular-momentum g-wave component incurs significant energetic penalties, rendering high-Tc superconductivity unlikely. We conclude that the absence of superconductivity in La2NiO4 arises from its robust intrinsic magnetism and the unfavorable pairing symmetry under pressure, suggesting that alternative routes-such as chemical doping or epitaxial strain-are necessary to suppress magnetism and unlock superconducting states.