Hydrogen induced electronic transition within correlated perovskite nickelates with heavy rare-earth composition

TL;DR

This study explores hydrogen-induced electronic transitions in heavy rare-earth nickelates, revealing non-monotonic resistivity changes and identifying middle rare-earth compositions as optimal for device applications.

Contribution

It extends understanding of hydrogen effects to heavier rare-earth nickelates, demonstrating non-reversible transitions in heavy compositions and highlighting the most suitable compositions for electronic devices.

Findings

Hydrogen induces non-monotonic resistivity changes across rare-earth series.

Heavy rare-earth nickelates show large resistivity changes but non-reversible transitions.

Middle rare-earth compositions are optimal for reversible hydrogen-induced electronic transitions.

Abstract

Although discovery in hydrogen induced electronic transition within perovskite family of rare-earth nickelate (ReNiO3) opens up a new paradigm in exploring both the new materials functionality and device applications, the existing research stays at ReNiO3 with light rare-earth compositions. To further extend the cognition towards heavier rare-earth, herein we demonstrate the hydrogen induced electronic transitions for quasi-single crystalline ReNiO3/LaAlO3 (001) heterostructures, covering a large variety of the rare-earth composition from Nd to Er. The hydrogen induced elevations in the resistivity of ReNiO3 (RH/R0) show an unexpected non-monotonic tendency with the atomic number of the rare-earth composition, e.g., firstly increase from Nd to Dy and afterwards decreases from Dy to Er. Although ReNiO3 with heavy rare-earth composition (e.g. DyNiO3) exhibits large RH/R0 up to 107, their hydrogen induced electronic transition is not reversible. Further probing the electronic structures via near edge X-ray absorption fine structure analysis clearly demonstrates the respective transition in electronic structures of ReNiO3 from Ni3+ based electron itinerant orbital configurations towards the Ni2+ based electron localized state. Balancing the hydrogen induced transition reversibility with the abruption in the variations of material resistivity, we emphasize that the ReNiO3 with middle rare-earth compositions (e.g. Sm) to be most suitable that caters for the potential applications in correlated electronic devices.