A superlattice approach to doping infinite-layer nickelates

TL;DR

This study introduces a superlattice method to achieve doping in infinite-layer nickelates, revealing reversible electronic changes and interfacial hole trapping, which advances understanding of doping mechanisms in transition metal oxides.

Contribution

The paper presents a novel superlattice synthesis and layer-selective reduction technique to control doping in nickelates, providing new insights into interfacial electronic configurations.

Findings

Doped holes are trapped at interfacial Ni sites.

Reversible electronic configuration changes upon reduction.

Electron doping results in uniform layer distribution.

Abstract

The recent observation of superconductivity in infinite-layer Nd$_{1-x}$Sr$_x$NiO$_2$ 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 LaNiO$_3$ embedded in insulating LaGaO$_3$, and used layer-selective topotactic reactions to reduce the nickelate layers to LaNiO$_{2}$. 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 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.