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Square‐planar coordinate Ni2+ ions in oxides are exclusively limited to a low‐spin state (S=0) owing to extensive crystal field splitting. Layered oxychalcogenides A2NiIIO2Ag2Se2 (A=Sr, Ba) with the S=1 NiO2 square lattice are now reported. The structural analysis revealed that the Ni2+ ion is under‐bonded by a significant tensile strain from neighboring Ag2Se2 layers, leading to the reduction in...
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