Direct observation of two-dimensional magnons in atomically thin CrI3

Cenker, John; Huang, Bevin; Suri, Nishchay; Thijssen, Pearl; Miller, Aaron; Song, Tiancheng; Taniguchi, Takashi; Watanabe, Kenji; McGuire, Michael A.; Xiao, Di; Xu, Xiaodong

doi:10.1038/s41567-020-0999-1

Title: Direct observation of two-dimensional magnons in atomically thin CrI₃

Abstract

Magnons are collective spin excitations in crystals with long-range magnetic order. The emergent van der Waals magnets provide a highly tunable platform to explore magnetic excitations in the two-dimensional limit with intriguing properties, manifesting from their honeycomb lattice structure and switchable magnetic configurations. Here, we report the direct observation of two-dimensional magnons through magneto-Raman spectroscopy with optical selection rules determined by the interplay between crystal symmetry, layer number and magnetic states in atomically thin CrI₃. In monolayers, we observe an acoustic magnon mode at ~0.3 meV. It has strict cross-circularly polarized selection rules locked to the magnetization direction that originates from the conservation of angular momentum of photons and magnons dictated by three-fold rotational symmetry. Additionally, we reveal optical magnon modes at ~17 meV. This mode is Raman silent in monolayers, but optically active in bilayers and bulk due to a relaxation of the parity criterion resulting from the layer index. In the layered antiferromagnetic states, we directly resolve two degenerate optical magnon modes with opposite angular momentum and conjugate optical selection rules. From these measurements, we quantitatively extract the spin-wave gap, magnetic anisotropy and intralayer and interlayer exchange constants, and establish two-dimensional magnets as a new platform for exploringmore » magnon physics.« less

Authors:

Cenker, John ^[1];

^[1]; Suri, Nishchay ^[2];

^[1]; Miller, Aaron ^[1];

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

^[3];

^[4];

^[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:: Mon Aug 10 00:00:00 EDT 2020

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

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1760125

Grant/Contract Number:: AC05-00OR22725

Resource Type:: Accepted Manuscript

Journal Name:: Nature Physics

Additional Journal Information:: Journal Volume: 17; Journal Issue: 1; Journal ID: ISSN 1745-2473

Publisher:: Nature Publishing Group (NPG)

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE

Citation Formats


                    Cenker, John, Huang, Bevin, Suri, Nishchay, Thijssen, Pearl, Miller, Aaron, Song, Tiancheng, Taniguchi, Takashi, Watanabe, Kenji, McGuire, Michael A., Xiao, Di, and Xu, Xiaodong. Direct observation of two-dimensional magnons in atomically thin CrI3.  United States: N. p., 2020. 
Web.  doi:10.1038/s41567-020-0999-1.

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                    Cenker, John, Huang, Bevin, Suri, Nishchay, Thijssen, Pearl, Miller, Aaron, Song, Tiancheng, Taniguchi, Takashi, Watanabe, Kenji, McGuire, Michael A., Xiao, Di, & Xu, Xiaodong. Direct observation of two-dimensional magnons in atomically thin CrI3.  United States.  https://doi.org/10.1038/s41567-020-0999-1

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                    Cenker, John, Huang, Bevin, Suri, Nishchay, Thijssen, Pearl, Miller, Aaron, Song, Tiancheng, Taniguchi, Takashi, Watanabe, Kenji, McGuire, Michael A., Xiao, Di, and Xu, Xiaodong. Mon .  
"Direct observation of two-dimensional magnons in atomically thin CrI3".  United States.  https://doi.org/10.1038/s41567-020-0999-1.  https://www.osti.gov/servlets/purl/1760125.

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@article{osti_1760125,

  title        = {Direct observation of two-dimensional magnons in atomically thin CrI3},

  author       = {Cenker, John and Huang, Bevin and Suri, Nishchay and Thijssen, Pearl and Miller, Aaron and Song, Tiancheng and Taniguchi, Takashi and Watanabe, Kenji and McGuire, Michael A. and Xiao, Di and Xu, Xiaodong},

  abstractNote = {Magnons are collective spin excitations in crystals with long-range magnetic order. The emergent van der Waals magnets provide a highly tunable platform to explore magnetic excitations in the two-dimensional limit with intriguing properties, manifesting from their honeycomb lattice structure and switchable magnetic configurations. Here, we report the direct observation of two-dimensional magnons through magneto-Raman spectroscopy with optical selection rules determined by the interplay between crystal symmetry, layer number and magnetic states in atomically thin CrI3. In monolayers, we observe an acoustic magnon mode at ~0.3 meV. It has strict cross-circularly polarized selection rules locked to the magnetization direction that originates from the conservation of angular momentum of photons and magnons dictated by three-fold rotational symmetry. Additionally, we reveal optical magnon modes at ~17 meV. This mode is Raman silent in monolayers, but optically active in bilayers and bulk due to a relaxation of the parity criterion resulting from the layer index. In the layered antiferromagnetic states, we directly resolve two degenerate optical magnon modes with opposite angular momentum and conjugate optical selection rules. From these measurements, we quantitatively extract the spin-wave gap, magnetic anisotropy and intralayer and interlayer exchange constants, and establish two-dimensional magnets as a new platform for exploring magnon physics.},

  doi          = {10.1038/s41567-020-0999-1},

  journal      = {Nature Physics},

  number       = 1,

  volume       = 17,

  place        = {United States},

  year         = {Mon Aug 10 00:00:00 EDT 2020},

  month        = {Mon Aug 10 00:00:00 EDT 2020}

}

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Title: Direct observation of two-dimensional magnons in atomically thin CrI3

Abstract

Citation Formats

Helicity-Changing Brillouin Light Scattering by Magnons in a Ferromagnetic Crystal journal, November 2019

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

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

Gigahertz Frequency Antiferromagnetic Resonance and Strong Magnon-Magnon Coupling in the Layered Crystal CrCl 3 journal, July 2019

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

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

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

Distinct magneto-Raman signatures of spin-flip phase transitions in CrI3 journal, August 2020

Theory of Antiferromagnetic Resonance journal, January 1952

Selection Rules for Light-Induced Magnetization of a Crystal with Threefold Symmetry: The Case of Antiferromagnetic NiO journal, January 2011

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

Relaxation Time of Terahertz Magnons Excited at Ferromagnetic Surfaces journal, August 2012

Temperature Dependence of Magnetic Excitations: Terahertz Magnons above the Curie Temperature journal, March 2017

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

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

Magnetic Order-Induced Polarization Anomaly of Raman Scattering in 2D Magnet CrI 3 journal, December 2019

Gate-tunable spin waves in antiferromagnetic atomic bilayers journal, June 2020

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

Probing magnetism in 2D materials at the nanoscale with single-spin microscopy journal, April 2019

Observation of Standing Spin Waves in a van der Waals Magnetic Material journal, November 2020

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

Evolution of interlayer and intralayer magnetism in three atomically thin chromium trihalides journal, May 2019

Topological magnons in CrI 3 monolayers: an itinerant fermion description journal, September 2020

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

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

On the origin of magnetic anisotropy in two dimensional CrI 3 journal, June 2017

Long-living terahertz magnons in ultrathin metallic ferromagnets journal, January 2015

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Title: Direct observation of two-dimensional magnons in atomically thin CrI₃

Helicity-Changing Brillouin Light Scattering by Magnons in a Ferromagnetic Crystal
journal, November 2019

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

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

Gigahertz Frequency Antiferromagnetic Resonance and Strong Magnon-Magnon Coupling in the Layered Crystal ${CrCl}_{3}$
journal, July 2019

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

Stacking tunable interlayer magnetism in bilayer ${CrI}_{3}$
journal, April 2019

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

Distinct magneto-Raman signatures of spin-flip phase transitions in CrI3
journal, August 2020

Theory of Antiferromagnetic Resonance
journal, January 1952

Selection Rules for Light-Induced Magnetization of a Crystal with Threefold Symmetry: The Case of Antiferromagnetic NiO
journal, January 2011

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

Relaxation Time of Terahertz Magnons Excited at Ferromagnetic Surfaces
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Temperature Dependence of Magnetic Excitations: Terahertz Magnons above the Curie Temperature
journal, March 2017

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

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journal, November 2016

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journal, December 2019

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journal, June 2020

Layer-dependent ferromagnetism in a van der Waals crystal down to the monolayer limit
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journal, April 2019

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journal, December 2017

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