Distinct spin–lattice and spin–phonon interactions in monolayer magnetic CrI3

Webster, Lucas; Liang, Liangbo; Yan, Jia-An

doi:10.1039/C8CP03599G

Distinct spin–lattice and spin–phonon interactions in monolayer magnetic CrI₃

Journal Article · Tue Aug 28 04:00:00 EDT 2018 · Physical Chemistry Chemical Physics. PCCP

DOI:https://doi.org/10.1039/C8CP03599G· OSTI ID:1474613

Webster, Lucas ^[1]; ^[2]; ^[1]

Towson University, MD (United States). Department of Physics, Astronomy, and Geosciences
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)

In this study, we apply the density-functional theory to study various phases (including non-magnetic (NM), anti-ferromagnetic (AFM), and ferromagnetic (FM)) in monolayer magnetic chromium triiodide (CrI₃), a recently fabricated 2D magnetic material. It is found that: (1) the introduction of magnetism in monolayer CrI₃ gives rise to metal-to-semiconductor transition; (2) the electronic band topologies as well as the nature of direct and indirect band gaps in either AFM or FM phases exhibit delicate dependence on the magnetic ordering and spin–orbit coupling; and (3) the phonon modes involving Cr atoms are particularly sensitive to the magnetic ordering, highlighting distinct spin–lattice and spin–phonon coupling in this magnet. First-principles simulations of the Raman spectra demonstrate that both frequencies and intensities of the Raman peaks strongly depend on the magnetic ordering. The polarization dependent A_1g modes at 77 cm^-1 and 130 cm^-1 along with the E_g mode at about 50 cm^-1 in the FM phase may offer a useful fingerprint to characterize this material. Lastly, our results not only provide a detailed guiding map for experimental characterization of CrI₃, but also reveal how the evolution of magnetism can be tracked by its lattice dynamics and Raman response.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1474613

Alternate ID(s):: OSTI ID: 1468663

Journal Information:: Physical Chemistry Chemical Physics. PCCP, Journal Name: Physical Chemistry Chemical Physics. PCCP Journal Issue: 36 Vol. 20; ISSN 1463-9076; ISSN PPCPFQ

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

References (52)

Density Functional Characterization of the Electronic Structure and Visible-Light Absorption of Cr-Doped Anatase TiO ₂ Yang, Kesong; Dai, Ying; Huang, Baibiao ChemPhysChem, Vol. 10, Issue 13 https://doi.org/10.1002/cphc.200900188	journal	September 2009
First principles phonon calculations in materials science Togo, Atsushi; Tanaka, Isao Scripta Materialia, Vol. 108 https://doi.org/10.1016/j.scriptamat.2015.07.021	journal	November 2015
Helicity-Resolved Raman Scattering of MoS ₂ , MoSe ₂ , WS ₂ , and WSe ₂ Atomic Layers Chen, Shao-Yu; Zheng, Changxi; Fuhrer, Michael S. Nano Letters, Vol. 15, Issue 4 https://doi.org/10.1021/acs.nanolett.5b00092	journal	March 2015
In-Plane Anisotropy in Mono- and Few-Layer ReS ₂ Probed by Raman Spectroscopy and Scanning Transmission Electron Microscopy Chenet, Daniel A.; Aslan, O. Burak; Huang, Pinshane Y. Nano Letters, Vol. 15, Issue 9 https://doi.org/10.1021/acs.nanolett.5b00910	journal	August 2015
Low-Frequency Interlayer Breathing Modes in Few-Layer Black Phosphorus Ling, Xi; Liang, Liangbo; Huang, Shengxi Nano Letters, Vol. 15, Issue 6 https://doi.org/10.1021/acs.nanolett.5b01117	journal	May 2015
Coupling and Stacking Order of ReS ₂ Atomic Layers Revealed by Ultralow-Frequency Raman Spectroscopy He, Rui; Yan, Jia-An; Yin, Zongyou Nano Letters, Vol. 16, Issue 2 https://doi.org/10.1021/acs.nanolett.5b04925	journal	January 2016
Atypical Exciton–Phonon Interactions in WS ₂ and WSe ₂ Monolayers Revealed by Resonance Raman Spectroscopy del Corro, E.; Botello-Méndez, A.; Gillet, Y. Nano Letters, Vol. 16, Issue 4 https://doi.org/10.1021/acs.nanolett.5b05096	journal	March 2016
Coupling of Crystal Structure and Magnetism in the Layered, Ferromagnetic Insulator CrI ₃ McGuire, Michael A.; Dixit, Hemant; Cooper, Valentino R. Chemistry of Materials, Vol. 27, Issue 2 https://doi.org/10.1021/cm504242t	journal	January 2015
Spin-Dependent Electron−Phonon Interaction in SmFeAsO by Low-Temperature Raman Spectroscopy Zhang, L.; Guan, P. F.; Feng, D. L. Journal of the American Chemical Society, Vol. 132, Issue 43 https://doi.org/10.1021/ja104847q	journal	November 2010
Discovery of intrinsic ferromagnetism in two-dimensional van der Waals crystals Gong, Cheng; Li, Lin; Li, Zhenglu Nature, Vol. 546, Issue 7657 https://doi.org/10.1038/nature22060	journal	April 2017
Layer-dependent ferromagnetism in a van der Waals crystal down to the monolayer limit Huang, Bevin; Clark, Genevieve; Navarro-Moratalla, Efrén Nature, Vol. 546, Issue 7657 https://doi.org/10.1038/nature22391	journal	June 2017
Reducing Dzyaloshinskii-Moriya interaction and field-free spin-orbit torque switching in synthetic antiferromagnets Chen, Ruyi; Cui, Qirui; Liao, Liyang Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-23414-3	journal	May 2021
Electric-field switching of two-dimensional van der Waals magnets Jiang, Shengwei; Shan, Jie; Mak, Kin Fai Nature Materials, Vol. 17, Issue 5 https://doi.org/10.1038/s41563-018-0040-6	journal	March 2018
Ligand-field helical luminescence in a 2D ferromagnetic insulator Seyler, Kyle L.; Zhong, Ding; Klein, Dahlia R. Nature Physics, Vol. 14, Issue 3 https://doi.org/10.1038/s41567-017-0006-7	journal	December 2017
Structural, electronic and vibrational properties of few-layer 2H- and 1T-TaSe2 Yan, Jia-An; Cruz, Mack A. Dela; Cook, Brandon Scientific Reports, Vol. 5, Issue 1 https://doi.org/10.1038/srep16646	journal	November 2015
Review on the Raman spectroscopy of different types of layered materials Zhang, Xin; Tan, Qing-Hai; Wu, Jiang-Bin Nanoscale, Vol. 8, Issue 12 https://doi.org/10.1039/C5NR07205K	journal	January 2016
Robust intrinsic ferromagnetism and half semiconductivity in stable two-dimensional single-layer chromium trihalides Zhang, Wei-Bing; Qu, Qian; Zhu, Peng Journal of Materials Chemistry C, Vol. 3, Issue 48 https://doi.org/10.1039/C5TC02840J	journal	January 2015
Raman intensities using time dependent density functional theory Van Caillie, Carole; Amos, Roger D. Physical Chemistry Chemical Physics, Vol. 2, Issue 10 https://doi.org/10.1039/a909807k	journal	January 2000
First-principles Raman spectra of MoS2, WS2 and their heterostructures Liang, Liangbo; Meunier, Vincent Nanoscale, Vol. 6, Issue 10 https://doi.org/10.1039/c3nr06906k	journal	January 2014
Phonon softening and crystallographic orientation of strained graphene studied by Raman spectroscopy Huang, M.; Yan, H.; Chen, C. Proceedings of the National Academy of Sciences, Vol. 106, Issue 18, p. 7304-7308 https://doi.org/10.1073/pnas.0811754106	journal	April 2009
The Raman effect in crystals Loudon, R. Advances in Physics, Vol. 50, Issue 7 https://doi.org/10.1080/00018730110101395	journal	November 2001
The Raman effect in crystals Loudon, R. Advances in Physics, Vol. 13, Issue 52 https://doi.org/10.1080/00018736400101051	journal	October 1964
Raman scattering of the model multiferroic oxide BiFeO ₃ : effect of temperature, pressure and stress Haumont, R.; Kreisel, J.; Bouvier, P. Phase Transitions, Vol. 79, Issue 12 https://doi.org/10.1080/01411590601067342	journal	December 2006
Raman scattering of the model multiferroic oxide BiFeO ₃ : effect of temperature, pressure and stress Haumont, R.; Kreisel, J.; Bouvier, P. Phase Transitions, Vol. 82, Issue 6 https://doi.org/10.1080/01411590902919357	journal	June 2009
Raman spectroscopy of atomically thin two-dimensional magnetic iron phosphorus trisulfide (FePS ₃ ) crystals Wang, Xingzhi; Du, Kezhao; Fredrik Liu, Yu Yang 2D Materials, Vol. 3, Issue 3 https://doi.org/10.1088/2053-1583/3/3/031009	journal	August 2016
Self-interaction correction to density-functional approximations for many-electron systems Perdew, J. P.; Zunger, Alex Physical Review B, Vol. 23, Issue 10, p. 5048-5079 https://doi.org/10.1103/PhysRevB.23.5048	journal	May 1981
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
From ultrasoft pseudopotentials to the projector augmented-wave method Kresse, G.; Joubert, D. Physical Review B, Vol. 59, Issue 3, p. 1758-1775 https://doi.org/10.1103/PhysRevB.59.1758	journal	January 1999
Theory of resonant Raman scattering of tetrahedral amorphous carbon Profeta, Mickael; Mauri, Francesco Physical Review B, Vol. 63, Issue 24 https://doi.org/10.1103/PhysRevB.63.245415	journal	June 2001
Anomalous phonon shifts in the paramagnetic phase of multiferroic R Mn 2 O 5 ( R = Bi , Eu, Dy): Possible manifestations of unconventional magnetic correlations García-Flores, A. F.; Granado, E.; Martinho, H. Physical Review B, Vol. 73, Issue 10 https://doi.org/10.1103/PhysRevB.73.104411	journal	March 2006
Probing the uniaxial strains in MoS 2 using polarized Raman spectroscopy: A first-principles study Doratotaj, Danna; Simpson, Jeffrey R.; Yan, Jia-An Physical Review B, Vol. 93, Issue 7 https://doi.org/10.1103/PhysRevB.93.075401	journal	February 2016
Strong magnetization and Chern insulators in compressed graphene / CrI 3 van der Waals heterostructures Zhang, Jiayong; Zhao, Bao; Zhou, Tong Physical Review B, Vol. 97, Issue 8 https://doi.org/10.1103/PhysRevB.97.085401	journal	February 2018
Raman spectrum of CrI 3 : An ab initio study Larson, Daniel T.; Kaxiras, Efthimios Physical Review B, Vol. 98, Issue 8 https://doi.org/10.1103/PhysRevB.98.085406	journal	August 2018
Resonant Raman scattering in YBa 2 Cu 3 O 7 : Band theory and experiment Heyen, E. T.; Rashkeev, S. N.; Mazin, I. I. Physical Review Letters, Vol. 65, Issue 24 https://doi.org/10.1103/PhysRevLett.65.3048	journal	December 1990
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Exchange Interaction Effects on the Optical Properties of L u M n O 3 Souchkov, A. B.; Simpson, J. R.; Quijada, M. Physical Review Letters, Vol. 91, Issue 2 https://doi.org/10.1103/PhysRevLett.91.027203	journal	July 2003
Temperature-dependent magnetic anisotropy in the layered magnetic semiconductors Cr I 3 and CrB r 3 Richter, Nils; Weber, Daniel; Martin, Franziska Physical Review Materials, Vol. 2, Issue 2 https://doi.org/10.1103/PhysRevMaterials.2.024004	journal	February 2018
Van der Waals engineering of ferromagnetic semiconductor heterostructures for spin and valleytronics Zhong, Ding; Seyler, Kyle L.; Linpeng, Xiayu Science Advances, Vol. 3, Issue 5 https://doi.org/10.1126/sciadv.1603113	journal	May 2017
Magnetoelectronics Prinz, G. A. Science, Vol. 282, Issue 5394 https://doi.org/10.1126/science.282.5394.1660	journal	November 1998
Discovery of Intrinsic Ferromagnetism in Two-Dimensional van der Waals Crystals Gong, Cheng; Li, Lin; Li, Zhenglu CLEO: Applications and Technology, Conference on Lasers and Electro-Optics https://doi.org/10.1364/cleo_at.2017.jth5c.2	conference	January 2017
Lattice dynamics of iron chalcogenides: Raman scattering study Opacic, Marko; Lazarevic, Nenad Journal of the Serbian Chemical Society, Vol. 82, Issue 9 https://doi.org/10.2298/JSC170321077O	journal	January 2017
Temperature-dependent magnetic anisotropy in the layered magnetic semiconductors CrI3 and CrBr3 Richter, Nils; Weber, Daniel; Martin, Franziska APS https://doi.org/10.25358/openscience-106	text	January 2018
Crystal and Magnetic Structures in Layered, Transition Metal Dihalides and Trihalides McGuire, Michael Crystals, Vol. 7, Issue 5 https://doi.org/10.3390/cryst7050121	journal	April 2017
First principles phonon calculations in materials science Togo, Atsushi; Tanaka, Isao arXiv https://doi.org/10.48550/arxiv.1506.08498	preprint	January 2015
Robust Intrinsic Ferromagnetism and Half Semiconductivity in Stable Two-Dimensional Single-Layer Chromium Trihalides Zhang, Wei-Bing; Qu, Qian; Zhu, Peng arXiv https://doi.org/10.48550/arxiv.1507.07275	text	January 2015
Coupling and stacking order of ReS2 atomic layers revealed by ultralow-frequency Raman spectroscopy He, Rui; Yan, Jia-An; Yin, Zongyon arXiv https://doi.org/10.48550/arxiv.1512.00092	text	January 2015
Layer-dependent Ferromagnetism in a van der Waals Crystal down to the Monolayer Limit Huang, Bevin; Clark, Genevieve; Navarro-Moratalla, Efren arXiv https://doi.org/10.48550/arxiv.1703.05892	text	January 2017
Van der Waals Engineering of Ferromagnetic Semiconductor Heterostructures for Spin and Valleytronics Zhong, Ding; Seyler, Kyle L.; Linpeng, Xiayu arXiv https://doi.org/10.48550/arxiv.1704.00841	text	January 2017
Crystal and Magnetic Structures in Layered, Transition Metal Dihalides and Trihalides McGuire, Michael A. arXiv https://doi.org/10.48550/arxiv.1704.08225	text	January 2017
Electric-field switching of two-dimensional van der Waals magnets Jiang, Shengwei; Shan, Jie; Mak, Kin Fai arXiv https://doi.org/10.48550/arxiv.1803.07272	text	January 2018
Theory of resonant Raman scattering of tetrahedral amorphous carbon Profeta, Mickael; Mauri, Francesco arXiv https://doi.org/10.48550/arxiv.cond-mat/0103028	text	January 2001
Exchange interaction effects on the optical properties of LuMnO3 Souchkov, A. B.; Simpson, J. R.; Drew, H. D. arXiv https://doi.org/10.48550/arxiv.cond-mat/0212644	text	January 2002

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Switching 2D magnetic states via pressure tuning of layer stacking Song, Tiancheng; Fei, Zaiyao; Yankowitz, Matthew Nature Materials, Vol. 18, Issue 12 https://doi.org/10.1038/s41563-019-0505-2	journal	October 2019
Tuning inelastic light scattering via symmetry control in the two-dimensional magnet CrI3 Huang, Bevin; Cenker, John; Zhang, Xiaoou Nature Nanotechnology, Vol. 15, Issue 3 https://doi.org/10.1038/s41565-019-0598-4	journal	January 2020
Electronic structure and magnetic properties of few-layer Cr ₂ Ge ₂ Te ₆ : the key role of nonlocal electron–electron interaction effects Menichetti, Guido; Calandra, Matteo; Polini, Marco 2D Materials, Vol. 6, Issue 4 https://doi.org/10.1088/2053-1583/ab2f06	journal	September 2019
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Proximity exchange effects in MoSe 2 and WSe 2 heterostructures with CrI 3 : Twist angle, layer, and gate dependence Zollner, Klaus; Faria Junior, Paulo E.; Fabian, Jaroslav Physical Review B, Vol. 100, Issue 8 https://doi.org/10.1103/physrevb.100.085128	journal	August 2019
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Electronic structure and magnetic properties of few-layer Cr$_2$Ge$_2$Te$_6$: the key role of nonlocal electron-electron interaction effects Menichetti, Guido; Calandra, Matteo; Polini, Marco arXiv https://doi.org/10.48550/arxiv.1904.10993	text	January 2019
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