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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 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,more » 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.« less

Authors:
ORCiD logo [1];  [1];  [2];  [1]; ORCiD logo [1];  [3]; ORCiD logo [3]; ORCiD logo [4];  [2]; ORCiD logo [1]
  1. Univ. of Washington, Seattle, WA (United States)
  2. Carnegie Mellon Univ., Pittsburgh, PA (United States)
  3. National Inst. for Materials Science, Tsukuba (Japan)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
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) (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.
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
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.
@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 = {Mon Jan 06 00:00:00 EST 2020},
month = {Mon Jan 06 00:00:00 EST 2020}
}

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Works referenced in this record:

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

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

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


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

  • Xi, Xiaoxiang; Zhao, Liang; Wang, Zefang
  • Nature Nanotechnology, Vol. 10, Issue 9, p. 765-769
  • DOI: 10.1038/nnano.2015.143

Probing Nanoscale Ferroelectricity by Ultraviolet Raman Spectroscopy
journal, September 2006

  • Tenne, D. A.; Bruchhausen, A.; Lanzillotti-Kimura, N. D.
  • Science, Vol. 313, Issue 5793
  • DOI: 10.1126/science.1130306

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