Heteroanionic Stabilization of Ni1+ with Nonplanar Coordination

Achievements

• Electronic structure calculations predict two new layered nickelate oxyfluoride materials derived from the Ruddlesden-Popper structure.
• The designed materials host Ni1+ in 4-coordinate square planar and 5-coordinate square pyramidal geometries, the latter enabled by the heteroanionic ligands.
• Predicted chemical reactions with high thermodynamic driving forces to guide the synthesis of these materials.

Significance. These new materials closely resemble undoped cuprate superconductors in their electronic structure. The approach of using heteroanionic materials (combining oxygen and fluorine) offers a new strategy for realizing cuprate-like physics in nickelates, which could lead to the discovery of new superconducting materials.

Relationship to IRG-2. The work establishes a promising new direction for the search of nickelate superconductors with potentially higher critical temperatures and offers heteroanionic synthesis strategies for experimental verification.