Unveiling the Interfacial Reconstruction Mechanism Enabling Stable Growth of the Delafossite PdCoO2 on Al2O3 and LaAlO3

TL;DR

This paper investigates how a secondary phase at the substrate surface enables the stable growth of PdCoO2 delafossite films on Al2O3 and LaAlO3, revealing a novel interfacial reconstruction mechanism crucial for high-quality thin film fabrication.

Contribution

It uncovers a new interfacial reconstruction mechanism involving a secondary phase that stabilizes PdCoO2 growth, differing from traditional strain relief processes.

Findings

Secondary phase stabilizes PdCoO2 films

Mechanism differs from conventional strain relief

Enables successful epitaxial growth on challenging substrates

Abstract

Delafossites, comprised of noble metal (A+) and strongly correlated sublayers (BO2-), form natural superlattices with highly anisotropic properties. These properties hold significant promise for various applications, but their exploitation hinges on the successful growth of high-quality thin films on suitable substrates. Unfortunately, the unique lattice geometry of delafossites presents a significant challenge to thin-film fabrication. Different delafossites grow differently, even when deposited on the same substrate, ranging from successful epitaxy to complete growth suppression. These variations often lack a clear correlation to obvious causes like lattice mismatch. Unidentified stabilization mechanisms appear to enable growth in certain cases, allowing these materials to form stable thin films or act as buffer layers for subsequent delafossite growth. This study employs advanced scanning transmission electron microscopy techniques to investigate the nucleation mechanism underlying the stable growth of PdCoO2 films on Al2O3 and LaAlO3 substrates, grown via molecular-beam epitaxy. Our findings reveal the presence of a secondary phase within the substrate surface that stabilizes the films. This mechanism deviates from the conventional understanding of strain relief mechanisms at oxide heterostructure interfaces and differs significantly from those observed for Cu-based delafossites.