Pressure and doping control of magnetic order and metallization in Ruddlesden-Popper La2NiO4

The discovery of superconductivity in multilayer nickelates under pressure has intensified interest in understanding the magnetic and electronic properties of Ruddlesden-Popper nickelates. Using density functional theory with Hubbard corrections, we investigate the magnetic ground state, electronic structure evolution under pressure, and Sr-doping effects in La${}_2$NiO${}_4$. We find that at ambient pressure, tetragonal La${}_2$NiO${}_4$ exhibits G-type antiferromagnetic order with negligible interlayer magnetic coupling. Under hydrostatic pressure, the system undergoes a continuous insulator-metal transition at ~50 GPa while maintaining robust magnetic order up to 75 GPa, contrasting sharply with the rapid magnetic suppression in La${}_3$Ni${}_2$O${}_7$. Sr doping induces a systematic evolution from G-type to A-type, to striped antiferromagnetic orders, and eventually to ferromagnetic order, accompanied by metallization. Furthermore, LaSrNiO${}_4$ displays weak charge and orbital orders. These results reveal the unique pressure and doping effects of single-layer nickelates and provide insights into the magnetic mechanisms underlying nickelate superconductivity.