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Title: Distinct magneto-Raman signatures of spin-flip phase transitions in CrI3

Abstract

The discovery of 2-dimensional (2D) materials, such as CrI3, that retain magnetic ordering at monolayer thickness has resulted in a surge of both pure and applied research in 2D magnetism. Here, we report a magneto-Raman spectroscopy study on multilayered CrI3, focusing on two additional features in the spectra that appear below the magnetic ordering temperature and were previously assigned to high frequency magnons. Instead, we conclude these modes are actually zone-folded phonons. We observe a striking evolution of the Raman spectra with increasing magnetic field applied perpendicular to the atomic layers in which clear, sudden changes in intensities of the modes are attributed to the interlayer ordering changing from antiferromagnetic to ferromagnetic at a critical magnetic field. Our work highlights the sensitivity of the Raman modes to weak interlayer spin ordering in CrI3.

Authors:
 [1];  [2];  [3];  [4];  [5]; ORCiD logo [3]; ORCiD logo [3];  [6]; ORCiD logo [7]; ORCiD logo [8]; ORCiD logo [9];  [9]; ORCiD logo [8]; ORCiD logo [6]; ORCiD logo [3];  [3]; ORCiD logo [3]; ORCiD logo [3]; ORCiD logo [1]
  1. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). Physical Measurement Lab. Nanoscale Device Characterization Division
  2. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). Physical Measurement Lab. Nanoscale Device Characterization Division; The Ohio State Univ., Columbus, OH (United States). Dept. of Physics
  3. The Ohio State Univ., Columbus, OH (United States). Dept. of Physics
  4. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). Physical Measurement Lab. Nanoscale Device Characterization Division; Towson Univ., Towson, MD (United States). Dept. of Physics, Astronomy and Geosciences
  5. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). Material Measurement Lab. Materials Measurement Science Division
  6. Pennsylvania State Univ., University Park, PA (United States). Dept. of Physics
  7. Univ. of Arkansas, Fayetteville, AR (United States). Dept. of Physics
  8. The Ohio State Univ., Columbus, OH (United States). Dept. of Chemistry and Biochemistry
  9. National Inst. for Materials Science, Tsukuba, Ibaraki (Japan)
Publication Date:
Research Org.:
Pennsylvania State Univ., University Park, PA (United States)
Sponsoring Org.:
USDOE Office of Science (SC); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division
OSTI Identifier:
1803544
Alternate Identifier(s):
OSTI ID: 1868539
Grant/Contract Number:  
SC0019068
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 11; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; 47 OTHER INSTRUMENTATION; Science & Technology; Other Topics; Ferromagnetism; Magnetic properties and materials; Magneto-optics; Two-dimensional materials

Citation Formats

McCreary, Amber, Mai, Thuc T., Utermohlen, Franz G., Simpson, Jeffrey R., Garrity, Kevin F., Feng, Xiaozhou, Shcherbakov, Dmitry, Zhu, Yanglin, Hu, Jin, Weber, Daniel, Watanabe, Kenji, Taniguchi, Takashi, Goldberger, Joshua E., Mao, Zhiqiang, Lau, Chun Ning, Lu, Yuanming, Trivedi, Nandini, Valdés Aguilar, Rolando, and Hight Walker, Angela R. Distinct magneto-Raman signatures of spin-flip phase transitions in CrI3. United States: N. p., 2020. Web. doi:10.1038/s41467-020-17320-3.
McCreary, Amber, Mai, Thuc T., Utermohlen, Franz G., Simpson, Jeffrey R., Garrity, Kevin F., Feng, Xiaozhou, Shcherbakov, Dmitry, Zhu, Yanglin, Hu, Jin, Weber, Daniel, Watanabe, Kenji, Taniguchi, Takashi, Goldberger, Joshua E., Mao, Zhiqiang, Lau, Chun Ning, Lu, Yuanming, Trivedi, Nandini, Valdés Aguilar, Rolando, & Hight Walker, Angela R. Distinct magneto-Raman signatures of spin-flip phase transitions in CrI3. United States. https://doi.org/10.1038/s41467-020-17320-3
McCreary, Amber, Mai, Thuc T., Utermohlen, Franz G., Simpson, Jeffrey R., Garrity, Kevin F., Feng, Xiaozhou, Shcherbakov, Dmitry, Zhu, Yanglin, Hu, Jin, Weber, Daniel, Watanabe, Kenji, Taniguchi, Takashi, Goldberger, Joshua E., Mao, Zhiqiang, Lau, Chun Ning, Lu, Yuanming, Trivedi, Nandini, Valdés Aguilar, Rolando, and Hight Walker, Angela R. Mon . "Distinct magneto-Raman signatures of spin-flip phase transitions in CrI3". United States. https://doi.org/10.1038/s41467-020-17320-3. https://www.osti.gov/servlets/purl/1803544.
@article{osti_1803544,
title = {Distinct magneto-Raman signatures of spin-flip phase transitions in CrI3},
author = {McCreary, Amber and Mai, Thuc T. and Utermohlen, Franz G. and Simpson, Jeffrey R. and Garrity, Kevin F. and Feng, Xiaozhou and Shcherbakov, Dmitry and Zhu, Yanglin and Hu, Jin and Weber, Daniel and Watanabe, Kenji and Taniguchi, Takashi and Goldberger, Joshua E. and Mao, Zhiqiang and Lau, Chun Ning and Lu, Yuanming and Trivedi, Nandini and Valdés Aguilar, Rolando and Hight Walker, Angela R.},
abstractNote = {The discovery of 2-dimensional (2D) materials, such as CrI3, that retain magnetic ordering at monolayer thickness has resulted in a surge of both pure and applied research in 2D magnetism. Here, we report a magneto-Raman spectroscopy study on multilayered CrI3, focusing on two additional features in the spectra that appear below the magnetic ordering temperature and were previously assigned to high frequency magnons. Instead, we conclude these modes are actually zone-folded phonons. We observe a striking evolution of the Raman spectra with increasing magnetic field applied perpendicular to the atomic layers in which clear, sudden changes in intensities of the modes are attributed to the interlayer ordering changing from antiferromagnetic to ferromagnetic at a critical magnetic field. Our work highlights the sensitivity of the Raman modes to weak interlayer spin ordering in CrI3.},
doi = {10.1038/s41467-020-17320-3},
journal = {Nature Communications},
number = 1,
volume = 11,
place = {United States},
year = {Mon Aug 03 00:00:00 EDT 2020},
month = {Mon Aug 03 00:00:00 EDT 2020}
}

Works referenced in this record:

Layer-dependent resonant Raman scattering of a few layer MoS 2 : Raman scattering of a few layer MoS
journal, September 2012

  • Chakraborty, Biswanath; Matte, H. S. S. Ramakrishna; Sood, A. K.
  • Journal of Raman Spectroscopy, Vol. 44, Issue 1
  • DOI: 10.1002/jrs.4147

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


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


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


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


Giant Anisotropic Raman Response of Encapsulated Ultrathin Black Phosphorus by Uniaxial Strain
journal, June 2016

  • Li, Yanyong; Hu, Zhixin; Lin, Shenghuang
  • Advanced Functional Materials, Vol. 27, Issue 19
  • DOI: 10.1002/adfm.201600986

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


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


Excited Excitonic States in 1L, 2L, 3L, and Bulk WSe 2 Observed by Resonant Raman Spectroscopy
journal, August 2014

  • del Corro, Elena; Terrones, Humberto; Elias, Ana
  • ACS Nano, Vol. 8, Issue 9
  • DOI: 10.1021/nn504088g

Lattice dynamics and phase transition in CrI 3 single crystals
journal, September 2018


First principles phonon calculations in materials science
journal, November 2015


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

Chemical accuracy for the van der Waals density functional
journal, December 2009

  • Klimeš, Jiří; Bowler, David R.; Michaelides, Angelos
  • Journal of Physics: Condensed Matter, Vol. 22, Issue 2
  • DOI: 10.1088/0953-8984/22/2/022201

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


Inhomogeneous Electron Gas
journal, November 1964


One Million Percent Tunnel Magnetoresistance in a Magnetic van der Waals Heterostructure
journal, July 2018


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


Restoring the Density-Gradient Expansion for Exchange in Solids and Surfaces
journal, April 2008


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


Intricate Resonant Raman Response in Anisotropic ReS 2
journal, September 2017


Identification of individual and few layers of WS2 using Raman Spectroscopy
journal, April 2013

  • Berkdemir, Ayse; Gutiérrez, Humberto R.; Botello-Méndez, Andrés R.
  • Scientific Reports, Vol. 3, Issue 1
  • DOI: 10.1038/srep01755

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


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

Soft self-consistent pseudopotentials in a generalized eigenvalue formalism
journal, April 1990


Magnetism in two-dimensional van der Waals materials
journal, October 2018


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

  • Kim, Hyun Ho; Yang, Bowen; Li, Siwen
  • Proceedings of the National Academy of Sciences, Vol. 116, Issue 23
  • DOI: 10.1073/pnas.1902100116

Raman Spectroscopy, Photocatalytic Degradation, and Stabilization of Atomically Thin Chromium Tri-iodide
journal, June 2018


Quasi-two-dimensional magnon identification in antiferromagnetic FeP S 3 via magneto-Raman spectroscopy
journal, February 2020


Boron nitride substrates for high-quality graphene electronics
journal, August 2010

  • Dean, C. R.; Young, A. F.; Meric, I.
  • Nature Nanotechnology, Vol. 5, Issue 10, p. 722-726
  • DOI: 10.1038/nnano.2010.172

Tunable metal–insulator transition in double-layer graphene heterostructures
journal, October 2011

  • Ponomarenko, L. A.; Geim, A. K.; Zhukov, A. A.
  • Nature Physics, Vol. 7, Issue 12
  • DOI: 10.1038/nphys2114

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


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


Combined cluster and atomic displacement expansion for solid solutions and magnetism
journal, May 2019


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


Advanced capabilities for materials modelling with Quantum ESPRESSO
journal, October 2017

  • Giannozzi, P.; Andreussi, O.; Brumme, T.
  • Journal of Physics: Condensed Matter, Vol. 29, Issue 46
  • DOI: 10.1088/1361-648X/aa8f79

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


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


Pseudopotentials for high-throughput DFT calculations
journal, January 2014


Self-Consistent Equations Including Exchange and Correlation Effects
journal, November 1965


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


Fundamental Spin Interactions Underlying the Magnetic Anisotropy in the Kitaev Ferromagnet CrI 3
journal, January 2020