Heterostructuring as Gateway to Electron Doping of Nickelate Superconductors
This study proposes a novel route to electron doping in nickelate superconductors through heterostructuring. First-principles calculations reveal that upon inserting wide-bandgap insulating layers of LaXO₃ (X = Al, Ga, Sc) into La₂NiO₄, the additional (LaO)⁺ layers act as electron donors, releasing carriers into the Ni-3d orbitals and thereby achieving disorder-free electron doping of Ruddlesden–Popper nickelates. This doping naturally places La₂NiO₄:La₂AlO₄ in the optimal regime for d_{x^2−y^2}-wave superconductivity, with many-body methods—including dynamical vertex approximation, fluctuation exchange, and dynamical cluster approximation—predicting a superconducting critical temperature exceeding 50 K and reaching as high as 127 K. The strategy circumvents the disorder typically introduced by conventional chemical doping, and is equally applicable to other nickelates such as La₃Ni₂O₇, offering a viable scheme for comprehensively mapping the electron-doping phase diagram of nickelates and extending the approach to other transition metal oxide systems.