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

Abstract

Layered 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 form, opening up opportunities for various functionalities 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 SHG and comparable to the SHG of the best (in terms of nonlinear susceptibility) two-dimensional nonlinear optical materials studied so far (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 antiferromagnetism. Finally, our results indicate that SHG is a highly sensitive probe of subtle magnetic ordersmore » and open up possibilities for the use of two-dimensional magnets in nonlinear and nonreciprocal optical devices.« less

Authors:
 [1];  [1];  [2];  [2];  [2];  [1];  [1];  [1];  [3];  [3]; ORCiD logo [4];  [5];  [6];  [3];  [7];  [2];  [3]
  1. Fudan Univ., Shanghai (China)
  2. Univ. of Washington, Seattle, WA (United States)
  3. Fudan Univ., Shanghai (China); Collaborative Innovation Center of Advanced Microstructures, Nanjing (China)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  5. Univ. of Washington, Seattle, WA (United States); Stanford Univ., CA (United States)
  6. Carnegie Mellon Univ. (CMU), Pittsburgh, PA (United States)
  7. Univ. of Hong Kong (China)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; National Natural Science Foundation of China (NSFC); National Basic Research Program of China; National Key Research and Development Program of China; National Science Foundation (NSF)
OSTI Identifier:
1649491
Grant/Contract Number:  
AC05-00OR22725; 11427902; 2014CB921601; 2016YFA0301002; SC0012509; NSF-DMR-1708419; 17303518P; 11622429
Resource Type:
Accepted Manuscript
Journal Name:
Nature (London)
Additional Journal Information:
Journal Name: Nature (London); Journal Volume: 572; Journal Issue: 7770; Journal ID: ISSN 0028-0836
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; magnetic properties and materials; nonlinear optics; two-dimensional materials

Citation Formats

Sun, Zeyuan, Yi, Yangfan, Song, Tiancheng, Clark, Genevieve, Huang, Bevin, Shan, Yuwei, Wu, Shuang, Huang, Di, Gao, Chunlei, Chen, Zhanghai, McGuire, Michael A., Cao, Ting, Xiao, Di, Tao Liu, Wei, Yao, Wang, Xu, Xiaodong, and Wu, Shiwei. Giant nonreciprocal second-harmonic generation from antiferromagnetic bilayer CrI3. United States: N. p., 2019. Web. https://doi.org/10.1038/s41586-019-1445-3.
Sun, Zeyuan, Yi, Yangfan, Song, Tiancheng, Clark, Genevieve, Huang, Bevin, Shan, Yuwei, Wu, Shuang, Huang, Di, Gao, Chunlei, Chen, Zhanghai, McGuire, Michael A., Cao, Ting, Xiao, Di, Tao Liu, Wei, Yao, Wang, Xu, Xiaodong, & Wu, Shiwei. Giant nonreciprocal second-harmonic generation from antiferromagnetic bilayer CrI3. United States. https://doi.org/10.1038/s41586-019-1445-3
Sun, Zeyuan, Yi, Yangfan, Song, Tiancheng, Clark, Genevieve, Huang, Bevin, Shan, Yuwei, Wu, Shuang, Huang, Di, Gao, Chunlei, Chen, Zhanghai, McGuire, Michael A., Cao, Ting, Xiao, Di, Tao Liu, Wei, Yao, Wang, Xu, Xiaodong, and Wu, Shiwei. Wed . "Giant nonreciprocal second-harmonic generation from antiferromagnetic bilayer CrI3". United States. https://doi.org/10.1038/s41586-019-1445-3. https://www.osti.gov/servlets/purl/1649491.
@article{osti_1649491,
title = {Giant nonreciprocal second-harmonic generation from antiferromagnetic bilayer CrI3},
author = {Sun, Zeyuan and Yi, Yangfan and Song, Tiancheng and Clark, Genevieve and Huang, Bevin and Shan, Yuwei and Wu, Shuang and Huang, Di and Gao, Chunlei and Chen, Zhanghai and McGuire, Michael A. and Cao, Ting and Xiao, Di and Tao Liu, Wei and Yao, Wang and Xu, Xiaodong and Wu, Shiwei},
abstractNote = {Layered 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 form, opening up opportunities for various functionalities 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 SHG and comparable to the SHG of the best (in terms of nonlinear susceptibility) two-dimensional nonlinear optical materials studied so far (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 antiferromagnetism. Finally, 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.},
doi = {10.1038/s41586-019-1445-3},
journal = {Nature (London)},
number = 7770,
volume = 572,
place = {United States},
year = {2019},
month = {7}
}

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Works referenced in this record:

Controlling magnetism in 2D CrI3 by electrostatic doping
journal, May 2018


Microscopic understanding of magnetic interactions in bilayer CrI 3
journal, March 2019


Discovery of intrinsic ferromagnetism in two-dimensional van der Waals crystals
journal, April 2017


Electric-field switching of two-dimensional van der Waals magnets
journal, March 2018


Gate-tunable room-temperature ferromagnetism in two-dimensional Fe3GeTe2
journal, October 2018


Two-dimensional itinerant ferromagnetism in atomically thin Fe3GeTe2
journal, August 2018


Stacking tunable interlayer magnetism in bilayer CrI 3
journal, April 2019


Stacking-Dependent Magnetism in Bilayer CrI 3
journal, November 2018


Effects of surface magnetism on optical second harmonic generation
journal, November 1991


Second Harmonic Generation and Magnetic-Dipole-Electric-Dipole Interference in Antiferromagnetic Cr 2 O 3
journal, October 1994


Nonlinear optical selection rule based on valley-exciton locking in monolayer ws2
journal, December 2015

  • Xiao, Jun; Ye, Ziliang; Wang, Ying
  • Light: Science & Applications, Vol. 4, Issue 12
  • DOI: 10.1038/lsa.2015.139

Electrical control of 2D magnetism in bilayer CrI3
journal, April 2018


Coupling of Crystal Structure and Magnetism in the Layered, Ferromagnetic Insulator CrI 3
journal, January 2015

  • McGuire, Michael A.; Dixit, Hemant; Cooper, Valentino R.
  • Chemistry of Materials, Vol. 27, Issue 2
  • DOI: 10.1021/cm504242t

Interplay between interlayer exchange and stacking in CrI3 bilayers
journal, September 2019


Electrical control of second-harmonic generation in a WSe2 monolayer transistor
journal, April 2015

  • Seyler, Kyle L.; Schaibley, John R.; Gong, Pu
  • Nature Nanotechnology, Vol. 10, Issue 5
  • DOI: 10.1038/nnano.2015.73

Probing magnetism in 2D van der Waals crystalline insulators via electron tunneling
journal, May 2018


Nonreciprocal responses from non-centrosymmetric quantum materials
journal, September 2018


Magnetoelectric and second-harmonic spectra in antiferromagnetic Cr 2 O 3
journal, April 1998

  • Muto, Makiko; Tanabe, Yukito; Iizuka-Sakano, Takako
  • Physical Review B, Vol. 57, Issue 16
  • DOI: 10.1103/PhysRevB.57.9586

Skyrmions in the Moiré of van der Waals 2D Magnets
journal, October 2018


Second-harmonic generation as a tool for studying electronic and magnetic structures of crystals: review
journal, January 2005

  • Fiebig, Manfred; Pavlov, Victor V.; Pisarev, Roman V.
  • Journal of the Optical Society of America B, Vol. 22, Issue 1
  • DOI: 10.1364/JOSAB.22.000096

Ising-Type Magnetic Ordering in Atomically Thin FePS 3
journal, November 2016


Strong room-temperature ferromagnetism in VSe2 monolayers on van der Waals substrates
journal, February 2018


Layer-dependent ferromagnetism in a van der Waals crystal down to the monolayer limit
journal, June 2017

  • Huang, Bevin; Clark, Genevieve; Navarro-Moratalla, Efrén
  • Nature, Vol. 546, Issue 7657
  • DOI: 10.1038/nature22391

Antiferromagnetic opto-spintronics
journal, March 2018


Room Temperature Intrinsic Ferromagnetism in Epitaxial Manganese Selenide Films in the Monolayer Limit
journal, April 2018


Optical second-harmonic generation from magnetized surfaces
journal, January 1989


Second harmonic microscopy of monolayer MoS 2
journal, April 2013


Probing Symmetry Properties of Few-Layer MoS 2 and h-BN by Optical Second-Harmonic Generation
journal, June 2013

  • Li, Yilei; Rao, Yi; Mak, Kin Fai
  • Nano Letters, Vol. 13, Issue 7
  • DOI: 10.1021/nl401561r

Giant tunneling magnetoresistance in spin-filter van der Waals heterostructures
journal, May 2018


Very large tunneling magnetoresistance in layered magnetic semiconductor CrI3
journal, June 2018


Second-Harmonic Light Generation in Crystals with Natural Optical Activity
journal, July 1968


Magnetization-induced-second-harmonic generation from surfaces and interfaces
journal, January 2005

  • Kirilyuk, Andrei; Rasing, Theo
  • Journal of the Optical Society of America B, Vol. 22, Issue 1
  • DOI: 10.1364/JOSAB.22.000148

Ligand-field helical luminescence in a 2D ferromagnetic insulator
journal, December 2017


Raman spectroscopy of atomically thin two-dimensional magnetic iron phosphorus trisulfide (FePS 3 ) crystals
journal, August 2016


    Works referencing / citing this record:

    Low-temperature monoclinic layer stacking in atomically thin CrI 3 crystals
    journal, November 2019


    Van der Waals engineering of magnetism
    journal, October 2019


    Electronic and magnetic properties of van der Waals ferromagnetic semiconductor VI 3
    journal, January 2020


    Tuning inelastic light scattering via symmetry control in the two-dimensional magnet CrI3
    journal, January 2020


    Switching 2D magnetic states via pressure tuning of layer stacking
    journal, October 2019


    Pressure-controlled interlayer magnetism in atomically thin CrI3
    journal, October 2019


    Van der Waals magnets: Wonder building blocks for two‐dimensional spintronics?
    journal, October 2019

    • Zhang, Wen; Wong, Ping Kwan Johnny; Zhu, Rui
    • InfoMat, Vol. 1, Issue 4
    • DOI: 10.1002/inf2.12048

    Linear Magnetoelectric Phase in Ultrathin MnPS 3 Probed by Optical Second Harmonic Generation
    journal, January 2020


    Quantum confinement-induced enhanced nonlinearity and carrier lifetime modulation in two-dimensional tin sulfide
    journal, January 2020


    Surface Nonlinear Optics on Centrosymmetric Dirac Nodal‐Line Semimetal ZrSiS
    journal, November 2019


    Probing and controlling magnetic states in 2D layered magnetic materials
    journal, September 2019


    Direct observation of van der Waals stacking–dependent interlayer magnetism
    journal, November 2019


    Controlled Growth and Thickness‐Dependent Conduction‐Type Transition of 2D Ferrimagnetic Cr 2 S 3 Semiconductors
    journal, December 2019