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The room temperature ferromagnetism in highly strained two-dimensional magnetic semiconductors

Dahai Wei

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 Corresponding author: Dahai Wei, dhwei@semi.ac.cn

DOI: 10.1088/1674-4926/44/4/040401

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In spintronics, it is still a challenge in experiments to realize the ferromagnetic semiconductors with Curie temperature Tc above room temperature. In 2017, the successful synthesis of two-dimensional (2D) van der Waals ferromagnetic semiconductors, including the monolayer CrI3 with Tc = 45 K[1] and the bilayer Cr2Ge2Te6 with Tc = 28 K[2] in experiments, has attracted extensive attention in the 2D ferromagnetic semiconductors. One of the key problems is to find suitable 2D magnetic semiconductors, which can have room-temperature operation as required in applications.

The physical properties of 2D materials are sensitive to external regulations, such as electric filed, stacking, heterostructure, strain, etc. The strain engineering is the powerful technique to change the lattice of materials, and thus control the electronic, magnetic, and various other physical properties of 2D materials. In contrast to bulk materials, 2D materials have stronger deformation capacity and thus can withstand greater elastic strain without fracture, which shows great advantages in strain engineering. For example, monolayer MoS2 can sustain strains as large as 11%[3], monolayer FeSe can sustain strains up to 6%[4, 5], and single-layer graphene can even withstand 25% elastic strain[6]. By density functional theory (DFT) calculations, it was predicted that the application of stain can dramatically change the Tc in various 2D magnetic semiconductors, including the monolayer Cr2Ge2Se6[7], the magnetic semiconductor heterostructure Cr2Ge2Te6/PtSe2[8], the 2D magnetic topological insulators Co3Sn3Se2, Co3Pb3S2, Co3Pb3Se2[9], the trilayer magnetic semiconductors CrI3 with different stacking orders[10], etc.

In a recent paper published in ACS Nano, Professor Yuerui Lu’s group at Australian National University and Professor Jan Seidel’s group at University of New South Wales Sydney have found the experiment evidence of room temperature ferromagnetism in highly strained nanoscale wrinkles in the 2D Cr2Ge2Te6[11]. Cr2Ge2Te6 is a layered van der Waals material, where the Tc of Cr2Ge2Te6 bulk is 61 K and the Tc of bilayer Cr2Ge2Te6 is about 28 K. The strained 2D Cr2Ge2Te6 is predicted to have ferromagnetism above room temperature according to some DFT calculations[7, 8]. In order to experimentally explore the effect of strain on Tc in 2D Cr2Ge2Te6, Professor Lu and Professor Seidel’s groups have systematically investigated the wrinkles of the 25 nm thick Cr2Ge2Te6 samples (about 36 layers), where the wrinkles are formed during the growth process. These wrinkles induce local strain in the materials, where the strain is dependent on the height and width of the formed wrinkle.

Fig. 1(a) shows the temperature-dependent magnetic force microscopy (MFM) signal of curved wrinkles in the 2D Cr2Ge2Te6 with 1.3% strain. The MFM has a magnetically coated tip near the sample surface, which is oscillated at resonance frequency. Because of the magnetic interactions between the tip and the sample, there will be a change in the oscillation phase, and this phase signal is recorded. When the measurement is taken at 4 K, the MFM signals show a stripe domain structure. At 80 K, the stripe pattern vanished in most of the areas, and the magnetic signals are left around the wrinkles. The strongest residual magnetic signal can be seen at the highest points. The higher areas should have higher strain values, because of the increased curvature resulting from the height difference. At 110 K, no more magnetic contrast can be detected, according to the vanish of the long-range magnetic order. Fig. 1(b) shows the temperature-dependent MFM signal of curved wrinkles in the 2D Cr2Ge2Te6 with 2.3% strain. The MFM signal persists at room temperature with a clear magnetic signal in wrinkles, leading to the experimental evidence of room temperature ferromagnetism.

Fig. 1.  (Color online) Temperature-dependent magnetic force microscopy (MFM) signal of curved wrinkles in the 2D Cr2Ge2Te6 with (a) 1.3% strain and (b) 2.3% stain in experiment. Numerically calculated Tc and the magnetic anisotropy energy (MAE) as a function of strain for (c) monolayer and (d) bilayer Cr2Ge2Te6, respectively. Adapted from Ref. [11].

In order to investigate the origin of the increased Tc with stain in the 2D Cr2Ge2Te6, Professor Bo Gu and Professor Gang Su’s group at University of Chinese Academy of Sciences have conducted the DFT calculations and the Monte Carlo simulations to study the Tc of monolayer and bilayer Cr2Ge2Te6 with strains[11]. Figs. 1(c) and 1(d) show the Tc and the magnetic anisotropy energy (MAE) as a function of strain for the monolayer and bilayer Cr2Ge2Te6, respectively. In both cases, the Tc of Cr2Ge2Te6 can be dramatically enhanced by the help of stain. For the bilayer Cr2Ge2Te6, the DFT results suggests that the room temperature ferromagnetic order is possible at 6%−8% strain. Since the Tc in strained bilayer Cr2Ge2Te6 is higher than Tc in stained monolayer Cr2Ge2Te6, it is expected that Tc in strained thick 2D Cr2Ge2Te6 can be even higher.

The enhancement of Tc with strain can be understood by the superexchange interaction, as categorized in the earlier reports by Professor Gu and Professor Su’s group[7-10]. The strain is expected to decrease the energy difference |EpEd| between the p orbitals of Te and the d orbitals of Cr, and thus increase the antiferromagnetic coupling, Jpd, between the p orbitals of Te and the d orbitals of Cr in 2D Cr2Ge2Te6. Due to the superexchange interaction, the enhanced Jpd can subsequently enhance the indirect ferromagnetic coupling between the d orbitals of Cr atoms, and finally enhance the Tc in 2D Cr2Ge2Te6.

This work provides experimental evidence of room temperature ferromagnetism in highly strained 2D magnetic semiconductor, and strong insight into the mechanism of the enhanced magnetism of Tc.



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O’Neill A, Rahman S, Zhang Z, et al. Enhanced room temperature ferromagnetism in highly strained 2D semiconductor Cr2Ge2Te6. ACS Nano, 2023, 17, 735 doi: 10.1021/acsnano.2c10209
Fig. 1.  (Color online) Temperature-dependent magnetic force microscopy (MFM) signal of curved wrinkles in the 2D Cr2Ge2Te6 with (a) 1.3% strain and (b) 2.3% stain in experiment. Numerically calculated Tc and the magnetic anisotropy energy (MAE) as a function of strain for (c) monolayer and (d) bilayer Cr2Ge2Te6, respectively. Adapted from Ref. [11].

[1]
Gong C, Li L, Li Z, et al. Discovery of intrinsic ferromagnetism in two-dimensional van der Waals crystals. Nature, 2017, 546, 265 doi: 10.1038/nature22060
[2]
Huang B, Clark G, Navarro-Moratalla E, et al. Layer-dependent ferromagnetism in a van der Waals crystal down to the monolayer limit. Nature, 2017, 546, 270 doi: 10.1038/nature22391
[3]
Bertolazzi S, Brivio J, Kis A. Stretching and breaking of ultrathin MoS2. ACS Nano, 2011, 5, 9703 doi: 10.1021/nn203879f
[4]
Peng R, Xu H C, Tan S Y, et al. Tuning the band structure and superconductivity in single-layer FeSe by interface engineering. Nat Commun, 2014, 5, 5044 doi: 10.1038/ncomms6044
[5]
Zhang P, Peng X L, Qian T, et al. Observation of high-TC superconductivity in rectangular FeSe/SrTiO3(110) monolayers. Phys Rev B, 2016, 94, 104510 doi: 10.1103/PhysRevB.94.104510
[6]
Cocco G, Cadelano E, Colombo L. Gap opening in graphene by shear strain. Phys Rev B, 2010, 81, 241412 doi: 10.1103/PhysRevB.81.241412
[7]
Dong X J, You J Y, Gu B, et al. Strain-induced room-temperature ferromagnetic semiconductors with large anomalous Hall conductivity in two-dimensional Cr2Ge2Se6. Phys Rev Appl, 2019, 12, 014020 doi: 10.1103/PhysRevApplied.12.014020
[8]
Dong X J, You J Y, Zhang Z, et al. Great enhancement of Curie temperature and magnetic anisotropy in two-dimensional van der Waals semiconductor heterostructures. Phys Rev B, 2020, 102, 144443 doi: 10.1103/PhysRevB.102.144443
[9]
Zhang Z, You J Y, Ma X Y, et al. Kagome quantum anomalous Hall effect with high Chern number and large band gap. Phys Rev B, 2021, 103, 014410 doi: 10.1103/PhysRevB.103.014410
[10]
Zhang Z, You J Y, Gu B, et al. Emergent magnetic states due to stacking and strain in the van der Waals magnetic trilayer CrI3. Phys Rev B, 2021, 104, 174433 doi: 10.1103/PhysRevB.104.174433
[11]
O’Neill A, Rahman S, Zhang Z, et al. Enhanced room temperature ferromagnetism in highly strained 2D semiconductor Cr2Ge2Te6. ACS Nano, 2023, 17, 735 doi: 10.1021/acsnano.2c10209
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    Dahai Wei. The room temperature ferromagnetism in highly strained two-dimensional magnetic semiconductors[J]. Journal of Semiconductors, 2023, 44(4): 040401. doi: 10.1088/1674-4926/44/4/040401
    D H Wei. The room temperature ferromagnetism in highly strained two-dimensional magnetic semiconductors[J]. J. Semicond, 2023, 44(4): 040401. doi: 10.1088/1674-4926/44/4/040401
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    Received: 30 January 2023 Revised: Online: Accepted Manuscript: 05 February 2023Uncorrected proof: 10 February 2023Published: 10 April 2023

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      Dahai Wei. The room temperature ferromagnetism in highly strained two-dimensional magnetic semiconductors[J]. Journal of Semiconductors, 2023, 44(4): 040401. doi: 10.1088/1674-4926/44/4/040401 ****D H Wei. The room temperature ferromagnetism in highly strained two-dimensional magnetic semiconductors[J]. J. Semicond, 2023, 44(4): 040401. doi: 10.1088/1674-4926/44/4/040401
      Citation:
      Dahai Wei. The room temperature ferromagnetism in highly strained two-dimensional magnetic semiconductors[J]. Journal of Semiconductors, 2023, 44(4): 040401. doi: 10.1088/1674-4926/44/4/040401 ****
      D H Wei. The room temperature ferromagnetism in highly strained two-dimensional magnetic semiconductors[J]. J. Semicond, 2023, 44(4): 040401. doi: 10.1088/1674-4926/44/4/040401

      The room temperature ferromagnetism in highly strained two-dimensional magnetic semiconductors

      DOI: 10.1088/1674-4926/44/4/040401
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      • Dahai Wei:received his B.S. (2004) at Nanjing University and Ph.D. (2010) at Fudan University. He was a post-doctor (2010–2012) at Tokyo University, a post-doctor and Humboldt Research Fellow (2012–2015) at Regensburg University. He has been a Professor at Institute of Semiconductors, Chinese Academy of Sciences since 2015. He is working on the of magnetic semiconductors and spintronics
      • Corresponding author: dhwei@semi.ac.cn
      • Received Date: 2023-01-30
      • Accepted Date: 2023-01-30
      • Available Online: 2023-02-05

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