Oxygen sublattice disorder and valence state modulation in infinite-layer nickelate superlattices

TL;DR

This study uses soft x-ray spectroscopy to explore how oxygen disorder and valence state changes at interfaces in nickelate superlattices influence their electronic properties and potential for high-temperature superconductivity.

Contribution

It demonstrates that interlayer material affects oxygen disorder and valence states, providing insights for designing nickelate-based superconductors.

Findings

Valence state and oxygen coordination modulate at interfaces.

Metallic conductivity depends on interlayer material.

Disorder in oxygen removal sites correlates with interlayer material.

Abstract

The family of infinite-layer nickelates promises important insights into the mechanism of unconventional superconductivity. Since superconductivity has so far only been observed in epitaxial thin films, heteroepitaxy with the substrate or a capping layer possibly plays an important role. Here, we use soft x-ray spectroscopy to investigate superlattices as a potential approach for a targeted material design of high-temperature superconductors. We observe modulations in valence state and oxygen coordination in topotactically reduced artificial superlattices with repeating interfaces between nickelate layers and layers of materials commonly used as substrates and capping layers. Our results show that depending on the interlayer material metallic conductivity akin to the parent infinite-layer compounds is achieved. Depth-resolved electronic structure measured by resonant x-ray reflectivity reveals a reconstructed ligand field and valence state at the interface, which is confined to one or two unit cells. The central layers show characteristics of monovalent nickel, but linear dichroism analysis reveals considerable disorder in the oxygen removal sites. We observe a quantitative correlation of this disorder with the interlayer material that is important for future modeling and design strategies.