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Article: Giant nonreciprocal second-harmonic generation from antiferromagnetic bilayer CrI3

TitleGiant nonreciprocal second-harmonic generation from antiferromagnetic bilayer CrI3
Authors
Keywordschromium
chromium triiodide
ferromagnetic material
molybdenum
molybdenum disulfide
Issue Date2019
PublisherNature Research (part of Springer Nature). The Journal's web site is located at http://www.nature.com/nature
Citation
Nature, 2019, v. 572 n. 7770, p. 497-512 How to Cite?
AbstractLayered antiferromagnetism is the spatial arrangement of ferromagnetic layers with antiferromagnetic interlayer coupling. The van der Waals magnet chromium triiodide (CrI3) has been shown to be a layered antiferromagnetic insulator in its few-layer form1, opening up opportunities for various functionalities2,3,4,5,6,7 in electronic and optical devices. Here we report an emergent nonreciprocal second-order nonlinear optical effect in bilayer CrI3. The observed second-harmonic generation (SHG; a nonlinear optical process that converts two photons of the same frequency into one photon of twice the fundamental frequency) is several orders of magnitude larger than known magnetization-induced SHG8,9,10,11 and comparable to the SHG of the best (in terms of nonlinear susceptibility) two-dimensional nonlinear optical materials studied so far12,13 (for example, molybdenum disulfide). We show that although the parent lattice of bilayer CrI3 is centrosymmetric, and thus does not contribute to the SHG signal, the observed giant nonreciprocal SHG originates only from the layered antiferromagnetic order, which breaks both the spatial-inversion symmetry and the time-reversal symmetry. Furthermore, polarization-resolved measurements reveal underlying C2h crystallographic symmetry—and thus monoclinic stacking order—in bilayer CrI3, providing key structural information for the microscopic origin of layered antiferromagnetism14,15,16,17,18. Our results indicate that SHG is a highly sensitive probe of subtle magnetic orders and open up possibilities for the use of two-dimensional magnets in nonlinear and nonreciprocal optical devices.
Persistent Identifierhttp://hdl.handle.net/10722/277121
ISSN
2019 Impact Factor: 42.778
2015 SCImago Journal Rankings: 21.936

 

DC FieldValueLanguage
dc.contributor.authorSun, Z-
dc.contributor.authorYi, Y-
dc.contributor.authorSong, T-
dc.contributor.authorClark, G-
dc.contributor.authorHuang, B-
dc.contributor.authorShan, Y-
dc.contributor.authorWu, S-
dc.contributor.authorHuang, D-
dc.contributor.authorGao, C-
dc.contributor.authorChen, Z-
dc.contributor.authorMcGuire, M-
dc.contributor.authorCao, T-
dc.contributor.authorXiao, D-
dc.contributor.authorLiu, WT-
dc.contributor.authorYao, W-
dc.contributor.authorXu, X-
dc.contributor.authorWu, S-
dc.date.accessioned2019-09-20T08:44:52Z-
dc.date.available2019-09-20T08:44:52Z-
dc.date.issued2019-
dc.identifier.citationNature, 2019, v. 572 n. 7770, p. 497-512-
dc.identifier.issn0028-0836-
dc.identifier.urihttp://hdl.handle.net/10722/277121-
dc.description.abstractLayered antiferromagnetism is the spatial arrangement of ferromagnetic layers with antiferromagnetic interlayer coupling. The van der Waals magnet chromium triiodide (CrI3) has been shown to be a layered antiferromagnetic insulator in its few-layer form1, opening up opportunities for various functionalities2,3,4,5,6,7 in electronic and optical devices. Here we report an emergent nonreciprocal second-order nonlinear optical effect in bilayer CrI3. The observed second-harmonic generation (SHG; a nonlinear optical process that converts two photons of the same frequency into one photon of twice the fundamental frequency) is several orders of magnitude larger than known magnetization-induced SHG8,9,10,11 and comparable to the SHG of the best (in terms of nonlinear susceptibility) two-dimensional nonlinear optical materials studied so far12,13 (for example, molybdenum disulfide). We show that although the parent lattice of bilayer CrI3 is centrosymmetric, and thus does not contribute to the SHG signal, the observed giant nonreciprocal SHG originates only from the layered antiferromagnetic order, which breaks both the spatial-inversion symmetry and the time-reversal symmetry. Furthermore, polarization-resolved measurements reveal underlying C2h crystallographic symmetry—and thus monoclinic stacking order—in bilayer CrI3, providing key structural information for the microscopic origin of layered antiferromagnetism14,15,16,17,18. Our results indicate that SHG is a highly sensitive probe of subtle magnetic orders and open up possibilities for the use of two-dimensional magnets in nonlinear and nonreciprocal optical devices.-
dc.languageeng-
dc.publisherNature Research (part of Springer Nature). The Journal's web site is located at http://www.nature.com/nature-
dc.relation.ispartofNature-
dc.rightsThis is a post-peer-review, pre-copyedit version of an article published in [insert journal title]. The final authenticated version is available online at: https://doi.org/[insert DOI]-
dc.subjectchromium-
dc.subjectchromium triiodide-
dc.subjectferromagnetic material-
dc.subjectmolybdenum-
dc.subjectmolybdenum disulfide-
dc.titleGiant nonreciprocal second-harmonic generation from antiferromagnetic bilayer CrI3-
dc.typeArticle-
dc.identifier.emailYao, W: wangyao@hku.hk-
dc.identifier.authorityYao, W=rp00827-
dc.description.naturelink_to_subscribed_fulltext-
dc.identifier.doi10.1038/s41586-019-1445-3-
dc.identifier.pmid31367036-
dc.identifier.scopuseid_2-s2.0-85069899258-
dc.identifier.hkuros305466-
dc.identifier.volume572-
dc.identifier.issue7770-
dc.identifier.spage497-
dc.identifier.epage512-
dc.publisher.placeUnited Kingdom-

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