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Chromium triiodide, CrI$_3$, is emerging as a promising magnetictwo-dimensional semiconductor where spins are ferromagnetically aligned withina single layer. Potential applications in spintronics arise from anantiferromagnetic ordering between adjacent layers that gives rise to spinfiltering and a large magnetoresistance in tunnelling devices. This key featureappears only in thin multilayers and it is not inherited from bulk crystals,where instead neighbouring layers share the same ferromagnetic spinorientation. This discrepancy between bulk and thin samples is unexpected, asmagnetic ordering between layers arises from exchange interactions that arelocal in nature and should not depend strongly on thickness. Here we solve thiscontroversy and show through polarization resolved Raman spectroscopy that thinmultilayers do not undergo a structural phase transition typical of bulkcrystals. As a consequence, a different stacking pattern is present in thin andbulk samples at the temperatures at which magnetism sets in and, according toprevious first-principles simulations, this results in a different interlayermagnetic ordering. Our experimental findings provide evidence for the stronginterplay between stacking order and magnetism in CrI$_3$, opening interestingperspectives to design the magnetic state of van der Waals multilayers.

Low-temperature monoclinic layer stacking in atomically thin CrI$_3$ crystals