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We examined what interactions control the sign and strength of the interlayercoupling in van der Waals ferromagnets such as Fe3-xGeTe2, Cr2Ge2Te6, CrI3 andVI3, to find that high-spin orbital interaction across the van der Waals gapsare a key to understanding their ferromagnetism. Interlayer ferromagneticcoupling in Fe3-xGeTe2 Cr2Ge2Te6, and CrI3 is governed by the high-spintwo-orbital two-electron destabilization, but that in VI3 by the high-spinfour-orbital two-electron stabilization. These interactions explain a number ofseemingly puzzling observations in van der Waals fer-romagnets.

High-spin orbital interactions across van der Waals gaps controlling the interlayer ferromagnetism in van der Waals ferromagnets