Tuning inelastic light scattering via symmetry control in the two-dimensional magnet CrI3

Huang, Bevin; Cenker, John; Zhang, Xiaoou; Ray, Essance L.; Song, Tiancheng; Taniguchi, Takashi; Watanabe, Kenji; McGuire, Michael A.; Xiao, Di; Xu, Xiaodong

doi:10.1038/s41565-019-0598-4

Title: Tuning inelastic light scattering via symmetry control in the two-dimensional magnet CrI₃

Abstract

The coupling between spin and charge degrees of freedom in a crystal gives rise to magneto-optical effects with applications in the sensitive detection of local magnetic order, optical modulation and data storage. In two-dimensional magnets these effects manifest themselves in the large magneto-optical Kerr effect, spontaneous helical light emission from ferromagnetic (FM) monolayers and electric-field induced Kerr rotation and giant second-order non-reciprocal optical effects in antiferromagnetic (AFM) bilayers. Here we demonstrate the tuning of inelastically scattered light through symmetry control in atomically thin chromium triiodide (CrI₃). In monolayers, we found an extraordinarily large magneto-optical Raman effect from an A_1g phonon mode due to the emergence of FM order. The linearly polarized, inelastically scattered light rotates by ~40°, more than two orders of magnitude larger than the rotation from the magneto-optical Kerr effect under the same experimental conditions. In CrI₃ bilayers, the same phonon mode becomes Davydov-split into two modes of opposite parity, which exhibit divergent selection rules that depend on inversion symmetry and the underlying magnetic order. We demonstrate the magneto-electrical control over these selection rules by activating or suppressing Raman activity for the odd-parity phonon mode and the magneto-optical rotation of scattered light from the even-parity phonon mode. Finally,more »« less

Authors:

^[1]; Cenker, John ^[1]; Zhang, Xiaoou ^[2]; Ray, Essance L. ^[1];

^[1]; Taniguchi, Takashi ^[3];

^[3];

^[4]; Xiao, Di ^[2];

^[1]

Univ. of Washington, Seattle, WA (United States)
Carnegie Mellon Univ., Pittsburgh, PA (United States)
National Inst. for Materials Science, Tsukuba (Japan)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Publication Date:: 2020-01-06

Research Org.:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; Ministry of Education, Culture, Sports, Science and Technology (MEXT), Japan

OSTI Identifier:: 1609042

Grant/Contract Number:: AC05-00OR22725; SC0012509; JP15K21722

Resource Type:: Accepted Manuscript

Journal Name:: Nature Nanotechnology

Additional Journal Information:: Journal Volume: 15; Journal Issue: 3; Journal ID: ISSN 1748-3387

Publisher:: Nature Publishing Group

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; ferromagnetism; magnetic properties and materials; two-dimensional materials

Citation Formats


                    Huang, Bevin, Cenker, John, Zhang, Xiaoou, Ray, Essance L., Song, Tiancheng, Taniguchi, Takashi, Watanabe, Kenji, McGuire, Michael A., Xiao, Di, and Xu, Xiaodong. Tuning inelastic light scattering via symmetry control in the two-dimensional magnet CrI3.  United States: N. p., 2020. 
Web.  doi:10.1038/s41565-019-0598-4.

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                    Huang, Bevin, Cenker, John, Zhang, Xiaoou, Ray, Essance L., Song, Tiancheng, Taniguchi, Takashi, Watanabe, Kenji, McGuire, Michael A., Xiao, Di, & Xu, Xiaodong. Tuning inelastic light scattering via symmetry control in the two-dimensional magnet CrI3.  United States.  https://doi.org/10.1038/s41565-019-0598-4

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                    Huang, Bevin, Cenker, John, Zhang, Xiaoou, Ray, Essance L., Song, Tiancheng, Taniguchi, Takashi, Watanabe, Kenji, McGuire, Michael A., Xiao, Di, and Xu, Xiaodong. Mon .  
"Tuning inelastic light scattering via symmetry control in the two-dimensional magnet CrI3".  United States.  https://doi.org/10.1038/s41565-019-0598-4.  https://www.osti.gov/servlets/purl/1609042.

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@article{osti_1609042,

  title        = {Tuning inelastic light scattering via symmetry control in the two-dimensional magnet CrI3},

  author       = {Huang, Bevin and Cenker, John and Zhang, Xiaoou and Ray, Essance L. and Song, Tiancheng and Taniguchi, Takashi and Watanabe, Kenji and McGuire, Michael A. and Xiao, Di and Xu, Xiaodong},

  abstractNote = {The coupling between spin and charge degrees of freedom in a crystal gives rise to magneto-optical effects with applications in the sensitive detection of local magnetic order, optical modulation and data storage. In two-dimensional magnets these effects manifest themselves in the large magneto-optical Kerr effect, spontaneous helical light emission from ferromagnetic (FM) monolayers and electric-field induced Kerr rotation and giant second-order non-reciprocal optical effects in antiferromagnetic (AFM) bilayers. Here we demonstrate the tuning of inelastically scattered light through symmetry control in atomically thin chromium triiodide (CrI3). In monolayers, we found an extraordinarily large magneto-optical Raman effect from an A1g phonon mode due to the emergence of FM order. The linearly polarized, inelastically scattered light rotates by ~40°, more than two orders of magnitude larger than the rotation from the magneto-optical Kerr effect under the same experimental conditions. In CrI3 bilayers, the same phonon mode becomes Davydov-split into two modes of opposite parity, which exhibit divergent selection rules that depend on inversion symmetry and the underlying magnetic order. We demonstrate the magneto-electrical control over these selection rules by activating or suppressing Raman activity for the odd-parity phonon mode and the magneto-optical rotation of scattered light from the even-parity phonon mode. Finally, our work underlines the unique opportunities provided by two-dimensional magnets to control the combined time-reversal and inversion symmetries to manipulate Raman optical selection rules and for exploring emergent magneto-optical effects and spin–phonon coupled physics.},

  doi          = {10.1038/s41565-019-0598-4},

  journal      = {Nature Nanotechnology},

  number       = 3,

  volume       = 15,

  place        = {United States},

  year         = {2020},

  month        = {1}

}

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Title: Tuning inelastic light scattering via symmetry control in the two-dimensional magnet CrI3

Abstract

Citation Formats

Raman spectrum of CrI 3 : An ab initio study journal, August 2018

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

Physical origin of giant excitonic and magneto-optical responses in two-dimensional ferromagnetic insulators journal, May 2019

Direct Photoluminescence Probing of Ferromagnetism in Monolayer Two-Dimensional CrBr 3 journal, March 2019

Amplitude Higgs mode in the 2 H − NbSe 2 superconductor journal, February 2014

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

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

Suppression of magnetic ordering in XXZ-type antiferromagnetic monolayer NiPS3 journal, January 2019

Chiral Spin Mode on the Surface of a Topological Insulator journal, September 2017

Enhancement of interlayer exchange in an ultrathin two-dimensional magnet journal, September 2019

Deterministic transfer of two-dimensional materials by all-dry viscoelastic stamping journal, April 2014

Gate-Controllable Magneto-optic Kerr Effect in Layered Collinear Antiferromagnets journal, December 2016

Distinct spin–lattice and spin–phonon interactions in monolayer magnetic CrI 3 journal, January 2018

Raman fingerprint of two terahertz spin wave branches in a two-dimensional honeycomb Ising ferromagnet journal, November 2018

Strongly enhanced charge-density-wave order in monolayer NbSe2 journal, July 2015

Probing Nanoscale Ferroelectricity by Ultraviolet Raman Spectroscopy journal, September 2006

Lattice Mode Degeneracy in Mo S 2 and Other Layer Compounds journal, August 1970

Magneto-elastic coupling in a potential ferromagnetic 2D atomic crystal journal, June 2016

Physical origin of Davydov splitting and resonant Raman spectroscopy of Davydov components in multilayer MoTe 2 journal, March 2016

Antiferromagnetic ordering in van der Waals 2D magnetic material MnPS 3 probed by Raman spectroscopy journal, July 2019

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

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

Giant nonreciprocal second-harmonic generation from antiferromagnetic bilayer CrI3 journal, July 2019

Deterministic transfer of two-dimensional materials by all-dry viscoelastic stamping preprint, January 2013

Strongly enhanced charge-density-wave order in monolayer NbSe$_2$ text, January 2015

Gate-controllable magneto-optic Kerr effect in layered collinear antiferromagnets text, January 2016

Layer-dependent Ferromagnetism in a van der Waals Crystal down to the Monolayer Limit text, January 2017

Chiral Spin Mode on the Surface of a Topological Insulator text, January 2017

Electrical Control of 2D Magnetism in Bilayer CrI3 text, January 2018

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Title: Tuning inelastic light scattering via symmetry control in the two-dimensional magnet CrI₃

Raman spectrum of ${CrI}_{3}$ : An $ab initio$ study
journal, August 2018

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

Physical origin of giant excitonic and magneto-optical responses in two-dimensional ferromagnetic insulators
journal, May 2019

Direct Photoluminescence Probing of Ferromagnetism in Monolayer Two-Dimensional CrBr ₃
journal, March 2019

Amplitude Higgs mode in the $2 H - {NbSe}_{2}$ superconductor
journal, February 2014

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

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

Suppression of magnetic ordering in XXZ-type antiferromagnetic monolayer NiPS3
journal, January 2019

Chiral Spin Mode on the Surface of a Topological Insulator
journal, September 2017

Enhancement of interlayer exchange in an ultrathin two-dimensional magnet
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Deterministic transfer of two-dimensional materials by all-dry viscoelastic stamping
journal, April 2014

Gate-Controllable Magneto-optic Kerr Effect in Layered Collinear Antiferromagnets
journal, December 2016

Distinct spin–lattice and spin–phonon interactions in monolayer magnetic CrI ₃
journal, January 2018

Raman fingerprint of two terahertz spin wave branches in a two-dimensional honeycomb Ising ferromagnet
journal, November 2018

Strongly enhanced charge-density-wave order in monolayer NbSe₂
journal, July 2015

Probing Nanoscale Ferroelectricity by Ultraviolet Raman Spectroscopy
journal, September 2006

Lattice Mode Degeneracy in Mo $S_{2}$ and Other Layer Compounds
journal, August 1970

Magneto-elastic coupling in a potential ferromagnetic 2D atomic crystal
journal, June 2016

Physical origin of Davydov splitting and resonant Raman spectroscopy of Davydov components in multilayer ${MoTe}_{2}$
journal, March 2016

Antiferromagnetic ordering in van der Waals 2D magnetic material MnPS ₃ probed by Raman spectroscopy
journal, July 2019

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

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

Giant nonreciprocal second-harmonic generation from antiferromagnetic bilayer CrI3
journal, July 2019

Deterministic transfer of two-dimensional materials by all-dry viscoelastic stamping
preprint, January 2013

Strongly enhanced charge-density-wave order in monolayer NbSe$_2$
text, January 2015

Gate-controllable magneto-optic Kerr effect in layered collinear antiferromagnets
text, January 2016

Layer-dependent Ferromagnetism in a van der Waals Crystal down to the Monolayer Limit
text, January 2017

Chiral Spin Mode on the Surface of a Topological Insulator
text, January 2017

Electrical Control of 2D Magnetism in Bilayer CrI3
text, January 2018

Electric-field switching of two-dimensional van der Waals magnets
text, January 2018

Suppression of magnetic ordering in XXZ-type antiferromagnetic monolayer NiPS3
text, January 2019

Direct photoluminescence probing of ferromagnetism in monolayer two-dimensional CrBr3
text, January 2019

Physical origin of giant excitonic and magneto-optical responses in two-dimensional ferromagnetic insulators
text, January 2019