Enhancement of interlayer exchange in an ultrathin two-dimensional magnet

Klein, Dahlia R.; MacNeill, David; Song, Qian; Larson, Daniel T.; Fang, Shiang; Xu, Mingyu; Ribeiro, R. A.; Canfield, P. C.; Kaxiras, Efthimios; Comin, Riccardo; Jarillo-Herrero, Pablo

doi:10.1038/s41567-019-0651-0

Enhancement of interlayer exchange in an ultrathin two-dimensional magnet

Journal Article · Mon Sep 16 00:00:00 EDT 2019 · Nature Physics

DOI:https://doi.org/10.1038/s41567-019-0651-0· OSTI ID:1562529

Klein, Dahlia R. ^[1]; MacNeill, David ^[1]; Song, Qian ^[1]; Larson, Daniel T. ^[2]; ^[2]; Xu, Mingyu ^[3]; ^[4]; Canfield, P. C. ^[3]; Kaxiras, Efthimios ^[2]; ^[1]; ^[1]

Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Harvard Univ., Cambridge, MA (United States)
Ames Lab., Ames, IA (United States); Iowa State Univ., Ames, IA (United States)
Ames Lab., Ames, IA (United States); Iowa State Univ., Ames, IA (United States); Universidade Federal do ABC, Santo André (Brazil)

Following the recent isolation of monolayer CrI₃, 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. In conclusion, 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.

View Accepted Manuscript (DOE)

Research Organization:: Ames Laboratory (AMES), Ames, IA (United States)

Sponsoring Organization:: Alfred P. Sloan Foundation; Gordon and Betty Moore Foundation; National Science Foundation (NSF); US Army Research Office (ARO); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-07CH11358; SC0018935

OSTI ID:: 1562529

Alternate ID(s):: OSTI ID: 1798973

Report Number(s):: IS--J-0,097; IS--J-9986

Journal Information:: Nature Physics, Journal Name: Nature Physics Journal Issue: 12 Vol. 15; ISSN 1745-2473

Publisher:: Nature Publishing Group (NPG)Copyright Statement

Country of Publication:: United States

Language:: English

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