Enhancement of interlayer exchange in an ultrathin two-dimensional magnet

DR Klein, D MacNeill, Q Song, DT Larson, S Fang… - Nature Physics, 2019 - nature.com
Nature Physics, 2019nature.com
Following the recent isolation of monolayer CrI3 (ref.), many more two-dimensional van der
Waals magnetic materials have been isolated,,,,,,,,,–. Their incorporation in van der Waals
heterostructures offers a new platform for spintronics,,,–, proximity magnetism and quantum
spin liquids. A primary question in this field is how exfoliating crystals to the few-layer limit
influences their magnetism. Studies of CrI3 have shown a different magnetic ground state for
ultrathin exfoliated films,, compared with the bulk, but the origin is not yet understood. Here …
Abstract
Following the recent isolation of monolayer CrI3 (ref. ), many more two-dimensional van der Waals magnetic materials have been isolated, , , , , , , , , –. Their incorporation in van der Waals heterostructures offers a new platform for spintronics, , , –, proximity magnetism and quantum spin liquids. A primary question in this field is how exfoliating crystals to the few-layer limit influences their magnetism. Studies of CrI3 have shown a different magnetic ground state for ultrathin exfoliated films,, compared with the bulk, but the origin is not yet understood. Here, we use electron tunnelling through few-layer crystals of the layered antiferromagnetic insulator CrCl3 to probe its magnetic order and find a tenfold enhancement of the interlayer exchange compared with bulk crystals. Moreover, temperature- and polarization-dependent Raman spectroscopy reveals that the crystallographic phase transition of bulk crystals does not occur in exfoliated films. This results in a different low-temperature stacking order and, we hypothesize, increased interlayer exchange. Our study provides insight into the connection between stacking order and interlayer interactions in two-dimensional magnets, which may be relevant for correlating stacking faults and mechanical deformations with the magnetic ground states of other more exotic layered magnets such as RuCl3 (ref. ).
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