High-Spin Orbital Interactions Across van der Waals Gaps Controlling the Interlayer Ferromagnetism in van der Waals Ferromagnets. 2022

Hyun-Joo Koo, and Reinhard K Kremer, and Myung-Hwan Whangbo
Department of Chemistry and Research Institute for Basic Sciences, Kyung Hee University, Seoul 02447, Republic of Korea.

We examined what interactions control the sign and strength of the interlayer coupling in van der Waals ferromagnets such as Fe3-GeTe2, Cr2Ge2Te6, CrI3, and VI3 to find that high-spin orbital interactions across the van der Waals gaps are a key to understanding their ferromagnetism. Interlayer ferromagnetic coupling in Fe3-GeTe2, Cr2Ge2Te6, and CrI3 is governed by the high-spin two-orbital two-electron destabilization, but that in VI3 by the high-spin four-orbital two-electron stabilization. These interactions explain a number of seemingly puzzling observations in van der Waals ferromagnets.

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