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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. Here we report layered oxychalcogenides A2NiO2Ag2Se2 (A = Sr, Ba) with the S = 1 NiO2 square lattice. The structural analysis revealed that the Ni2+ ion is underbonded by a significant tensile strain from neighboring Ag2Se2 layers, leading to a reduction of the crystal field energy. Ba2NiO2Ag2Se2 exhibits a G-type spin order at 130 K, indicating fairly strong in-plan interactions. The high-pressure synthesis employed here possibly assists the expansion of NiO2 square lattice by taking the advantage of a difference in compressibility in oxide and selenide layers.
Matsumoto, Y.
, Yamamoto, T.
, Nakano, K.
, Takatsu, H.
, Murakami, T.
, Hongo, K.
, Maezono, R.
, Ogino, H.
, Song, D.
, Brown, C.
, Cedric, T.
and Kageyama, H.
(2019),
High-Pressure Synthesis of A<sub>2</sub>NiO<sub>2</sub>Ag<sub>2</sub>Se<sub>2</sub> (A=Sr, Ba) with a High-Spin Ni<sup>2+</sup> in Square-Planar Coordination, Angewandte Chemie-International Edition, [online], https://tsapps.nist.gov/publication/get_pdf.cfm?pub_id=927211
(Accessed October 28, 2025)