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Following the recent isolation of monolayer CrI3, there has been a surge ofnew two-dimensional van der Waals magnetic materials, whose incorporation invan der Waals heterostructures offers a new platform for spintronics, proximitymagnetism, and quantum spin liquids. A primary question in this burgeoningfield is how exfoliating crystals to the few-layer limit influences theirmagnetism. Studies on CrI3 have shown a different magnetic ground state forultrathin exfoliated films but the origin is not yet understood. Here, we useelectron tunneling through few-layer crystals of the layered antiferromagneticinsulator CrCl3 to probe its magnetic order, finding a ten-fold enhancement inthe interlayer exchange compared to bulk crystals. Moreover, temperature- andpolarization-dependent Raman spectroscopy reveal that the crystallographicphase transition of bulk crystals does not occur in exfoliated films. Thisresults in a different low temperature stacking order and, we hypothesize,increased interlayer exchange. Our study provides new insight into theconnection between stacking order and interlayer interactions in noveltwo-dimensional magnets, which may be relevant for correlating stacking faultsand mechanical deformations with the magnetic ground states of other moreexotic layered magnets, such as RuCl3.

Giant enhancement of interlayer exchange in an ultrathin 2D magnet