Magnetic and electronic properties of layered Sr2NiO2Cl2 with square planar coordination

Abstract

Local coordination geometry is crucial in determining the physical properties of transition metal compounds. In this work, we report a detailed density functional theory study on the magnetic and electronic properties of layered Sr2NiO2Cl2, which possesses an unusual square planar coordination. Due to the crystal field and spin splitting, Ni 3d electrons fully occupy the dxz, dyz, and dxy orbitals, while partially occupy the dz2 and dx2-y2 states, leading to the high spin state of Ni2+ ions and strong antiferromagnetic in-plane nearest-neighbor exchange interaction J1. Thus, Sr2NiO2Cl2 is predicted to exhibit a G-type magnetic ground state, which all nearest-neighbor magnetic moments are antiparallel to each other in the NiO2 plane. A band gap is opened irrespective of the specific magnetic state since the unique square planar crystal field splitting. Finally, large orbital moments and giant easy-plane magnetocrystalline anisotropy energy are obtained, which is again related to the unique coordination environment.