Stabilization of Tetragonal Phase and Aluminum-Doping Effect in a Bilayer Nickelate

Recent studies suggest that the tetragonal phase of the Ruddlesden-Popper (RP) bilayer nickelate, La3Ni2O7 or La2PrNi2O7, which is stabilized under high pressures, is responsible for high-temperature superconductivity (HTSC). In this context, realization of the tetragonal phase at ambient pressure could be a rational step to achieve the goal of ambient-pressure HTSC in the nickelate system. By employing the concept of Goldschmidt tolerance factor, we succeed in stabilizing the tetragonal phase by aluminum doping together with post annealing under moderately high oxygen pressure. X-ray and neutron diffractions verify the tetragonal I4/mmm structure for the post-annealed samples La3Ni2−xAlxO7−δ (0.3 ≤ x ≤ 0.5). The Al-doped samples, including the tetragonal ones, show semiconducting properties, carry localized magnetic moments, and exhibit spin-glass-like behaviors at low temperatures, all of which can be explained in terms of charge carrier localization. Furthermore, high-pressure resistance measurements on post-annealed samples reveal that even a low Al doping (x = 0.05) suppresses superconductivity almost completely. This work gives information about the effect of nonmagnetic impurity on metallicity as well as superconductivity in bilayer nickelates, which would contribute to understanding the superconducting mechanism in RP nickelates.