Single-Layer T'; Nickelates: Synthesis of the La and Pr Members and Electronic Properties across the Rare-Earth Series

Understanding high-temperature unconventional superconductivity has become a long-lasting problem in which the cuprates stand as central reference materials. Given this impasse, the recent discovery of superconductivity in analogous nickelate thin films represents a fundamental breakthrough calling for the identification of additional materials in this class. In particular, thermodynamically more robust systems are required to upgrade nickelate superconductors from thin films to bulk samples. Here, we contribute in this direction by reporting the synthesis of the new single-layer T' Pr2NiO3F compound, assessing this synthesis in relation to the only previous T' nickelate La2NiO3F, and analyzing the electronic properties across the R2NiO3F series (R = La-Lu) via first-principles calculations. We find that these mixed anion systems have a comparatively high degree of stability and their synthesis enables a fine-tuning of their composition as inferred from their characterization. Furthermore, we find that these unprecedented square-planar nickelates hold great promise as prospective superconductors due to their exceptional electronic structure.

Automated summary

Understanding high-temperature unconventional superconductivity has always been a long-standing problem, with cuprates as central reference materials. The recent discovery of superconductivity in analogous nickelate thin films marks a fundamental breakthrough, calling for the search of additional materials in this class. In this study, a new single-layer T' Pr2NiO3F compound was synthesized and compared with the previously synthesized T' nickelate La2NiO3F. The electronic properties of the R2NiO3F series (R = La-Lu) were analyzed using first-principles calculations. The mixed anion systems were found to have a high degree of stability, and their composition could be finely tuned through synthesis. Furthermore, these unprecedented square-planar nickelates show great promise as potential superconductors due to their exceptional electronic structure.