Superlattice approach to doping infinite-layer nickelates

The recent observation of superconductivity in infinite-layer Nd1-xSrxNiO2 thin films has attracted a lot of attention, since this compound is electronically and structurally analogous to the superconducting cuprates. Due to the challenges in the phase stabilization upon chemical doping with Sr, we synthesized artificial superlattices of LaNiO3 embedded in insulating LaGaO3, and we used layer-selective topotactic reactions to reduce the nickelate layers to LaNiO2. Hole doping is achieved via interfacial oxygen atoms and tuned via the layer thickness. We used electrical transport measurements, transmission electron microscopy, and x-ray spectroscopy together with ab initio calculations to track changes in the local nickel electronic configuration upon reduction, and we found that these changes are reversible. Our experimental and theoretical data indicate that the doped holes are trapped at the interfacial quadratic pyramidal Ni sites. Calculations for electron-doped cases predict a different behavior, with evenly distributed electrons among the layers, thus opening up interesting perspectives for interfacial doping of transition-metal oxides