Two-Dimensional Janus Alloys for Spintronics on the Example of Fe₂I₃Br₃

Abstract

Two-dimensional (2D) Janus monolayers with mirror asymmetry have exceptional physical properties. This means that they can be used in next-generation optoelectronic, electronic, and electromechanical devices. Thе article presents a first-principles study of the electronic and magnetic properties of the 2D Janus monolayer Fe₂I₃Br₃ using density functional theory. A crystallographic model of the Fe₂I₃Br₃ Janus alloy has been created, its equilibrium structure has been calculated, and its electronic, magnetic, and mechanical properties have been determined. It is shown that the 2D Janus monolayers of Fe₂I₃Br₃ are dynamically and thermodynamically stable, as evidenced by the results of calculations of phonon spectra and formation energies, and also demonstrate a semiconductor nature. The band structure of Fe₂I₃Br₃ has a spin-polarized antiferromagnetic ordering with a band gap of about 1 eV. The Neel temperature was 75 K. In materials of this type, it is possible to realize states that are difficult or practically impossible to obtain in bulk magnetic samples. The results obtained can contribute to the development of science about two-dimensional functional materials, which will find application in various fields of the nanotechnology industry

The results were obtained using the equipment of Shared Resource Center "Far Eastern Computing Resource" IACP FEB RAS (https://www.cc.dvo.ru). The work was supported by the Russian Science Foundation (project no. 25-23-20239)

Please cite this article in English as:

Medintseva T.V., Kartsev A.I., Tarasov Yu.I. Two-dimensional Janus alloys for spintronics on the example of Fe₂I₃Br₃. Herald of the Bauman Moscow State Technical University, Series Natural Sciences, 2026, no. 3 (126), pp. 40--52 (in Russ.). EDN: LMUUFH

References

[1] Negedu S.D., Kartsev A., Palit M., et al. Energy harvesting from atomically thin Co₂Te₃. J. Phys. Chem. C, 2022, vol. 126, iss. 30, pp. 12545--12553. DOI: https://doi.org/10.1021/acs.jpcc.2c02102

[2] Gowda C.C., Kartsev A., Tiwari N., et al. Harvesting magneto-acoustic waves using magnetic two-dimensional chromium telluride (CrTe₃). arXiv:2406.15029. DOI: https://doi.org/10.48550/arXiv.2406.15029

[3] Gowda C.C., Kartsev A., Tiwari N., et al. Non-thermal magnetic deicing using two-dimensional chromium telluride. J. Mater. Chem. C, 2024, vol. 12, iss. 46, pp. 18691--18703. DOI: https://doi.org/10.1039/D4TC02542C

[4] Rassekh M., He J., Shayesteh S.F., et al. Remarkably enhanced curie temperature in monolayer cri3 by hydrogen and oxygen adsorption: a first-principles calculations. Comput. Mater. Sci., 2020, vol. 183, art. 109820. DOI: https://doi.org/10.1016/j.commatsci.2020.109820

[5] Wang Z., Gutierrez Lezama I., Ubrig N., et al. Very large tunneling magnetoresistance in layered magnetic semiconductor CrI₃. Nat. Commun., 2018, vol. 9, art. 2516. DOI: https://doi.org/10.1038/s41467-018-04953-8

[6] Yue W., Shan J., Jiao R., et al. Strain-controlled electronic and magnetic properties of Janus nitride MXene monolayer MnCrNO₂. Appl. Sci., 2024, vol. 14, iss. 18, art. 8427. DOI: https://doi.org/10.3390/app14188427

[7] Huynh T.P.T., Vo V.O., Guerrero-Sanchez J., et al. Effects of vacancy and Ge substitution in Janus Si₂PAs monolayer: site-dependent electronic and magnetic properties. Appl. Phys. A, 2024, vol. 130, no. 8, art. 571. DOI: https://doi.org/10.1007/s00339-024-07719-w

[8] Trinh T.H., Ha C.V., Guerrero-Sanchez J., et al. Electronic and magnetic properties of Janus ZrSSe monolayer doped with V impurity and VX₃ (X = C, N, O, and F) clusters. Phys. Scr., 2024, vol. 99, art. 105942. DOI: https://doi.org/10.1088/1402-4896/ad7421

[9] Ren K., Wang K., Zhang G. Atomic adsorption-controlled magnetic properties of a two-dimensional (2D) Janus monolayer. ACS Appl. Electron. Mater., 2022, vol. 4, iss. 9, pp. 4689--4697. DOI: https://doi.org/10.1021/acsaelm.2c00740

[10] Wu Y.-L., Zeng Z.-Y., Geng H.-Y., et al. Electronic structures and magnetic properties of Janus NbSSe monolayer controlled by carrier doping. J. Appl. Phys., 2024, vol. 136, no. 9, art. 093904. DOI: https://doi.org/10.1063/5.0231503

[11] Rimmler B.H., Pal B., Parkin S.S.P. Non-collinear antiferromagnetic spintronics. Nat. Rev. Mater., 2025, vol. 10, pp. 109--127. DOI: https://doi.org/10.1038/s41578-024-00706-w

[12] Shi J., Arpaci S., Lopez-Dominguez V., et al. Electrically controlled all-antiferro-magnetic tunnel junctions on silicon with large room-temperature magnetoresistance. Adv. Mater., 2024, vol. 36, art. 2312008. DOI: https://doi.org/10.1002/adma.202312008

[13] Chen H., Liu L., Zhou X., et al. Emerging antiferromagnets for spintronics. Adv. Mater., 2024, vol. 36, no. 14, art. 2310379. DOI: https://doi.org/10.1002/adma.202310379

[14] Shao D.F., Tsymbal E.Y. Antiferromagnetic tunnel junctions for spintronics. npj Spintronics, 2024, vol. 2, art. 13. DOI: https://doi.org/10.1038/s44306-024-00014-7

[15] Xu F., Dai S., Cen W., et al. Study on the piezoelectric properties and the mechanism of strain-regulated piezoelectricity in flexible Janus monolayers Cr₂X₃Y₃ (X/Y = Cl, Br, I). Phys. Scr., 2024, vol. 99, no. 2, art. 025987. DOI: https://doi.org/10.1088/1402-4896/ad1da0

[16] Zhang F., Mi W., Wang X. Spin-dependent electronic structure and magnetic anisotropy of 2D ferromagnetic Janus Cr₂I₃X₃ (X = Br, Cl) monolayers. Adv. Electron. Mater., 2020, vol. 6, no. 1, art. 1900778. DOI: https://doi.org/10.1002/aelm.201900778

[17] Ghobadi N., Gholami S., Soleimani-Amiri S. Electronic, spintronic, and piezoelectric properties of new Janus ZnAXY (A = Si, Ge, Sn; X, Y = S, Se, Te) monolayers. Phys. Rev. B, 2023, vol. 107, art. 075443. DOI: https://doi.org/10.1103/PhysRevB.107.075443

[18] Zeng H., Jin S., Wang J., et al. Ferromagnetic half-metal with high curie temperature: Janus Mn2PAs monolayer. J. Mater. Sci., 2021, vol. 56, iss. 23, pp. 13215--13226. DOI: https://doi.org/10.1007/s10853-021-06158-9

[19] Xu H.-Q., Xiao G., Xiao W.-Z., et al. Piezoelectricity and optical properties of Janus MXY (M = Sb, As; X = Te, Se; Y = Br, I) monolayers. Micro Nanostruct., 2022, vol. 170, art. 207396. DOI: https://doi.org/10.1016/j.micrna.2022.207396

[20] Yang Q., Wang D., Zeng Z.-Y., et al. High-performance photocatalytic and piezoelectric properties of two-dimensional transition metal oxyhalide ZrOX₂ (X = Br, I) and their Janus structures. Phys. Rev. B, 2024, vol. 109, art. 035411. DOI: https://doi.org/10.1103/PhysRevB.109.035411

[21] Monkhorst H.J., Pack J.D. Special points for Brillouin-zone integrations. Phys. Rev. B, 1976, vol. 13, no. 12, pp. 5188--5192. DOI: https://doi.org/10.1103/PhysRevB.13.5188

[22] Grimme S., Antony J., Ehrlich S., et al. A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H--Pu. J. Chem. Phys., 2010, vol. 132, iss. 15, art. 154104. DOI: https://doi.org/10.1063/1.3382344

[23] Grimme S., Ehrlich S., Goerigk L. Effect of the damping function in dispersion corrected density functional theory. J. Comput. Chem., 2011, vol. 32, iss. 7, pp. 1456--1465. DOI: https://doi.org/10.1002/jcc.21759

[24] Bader R.F.W. Atoms in molecules: a quantum theory. Oxford Univ. Press, 1991.

[25] Becke A.D., Edgecombe K.E. A simple measure of electron localization in atomic and molecular systems. J. Chem. Phys., 1990, vol. 92, iss. 9, pp. 5397--5403. DOI: https://doi.org/10.1063/1.458517

[26] Tang W., Sanville E., Henkelman G. A grid-based Bader analysis algorithm without lattice bias. J. Phys.: Condens. Matter, 2009, vol. 21, iss. 8, art. 084204. DOI: https://doi.org/10.1088/0953-8984/21/8/084204

[27] Kartsev A., Obraztsov K., Lega P. Magnetic properties of metal dichalcogenide in the frame of Heisenberg-like model: DFT and Monte-Carlo methods. J. Commun. Technol. Electron., 2023, vol. 68, no. 10, pp. 1169--1190. DOI: https://doi.org/10.1134/S1064226923100054

[28] Kartsev A., Malkovsky S., Chibisov A. Analysis of ionicity-magnetism competition in 2D-MX3 halides towards a low-dimensional materials study based on GPU-enabled computational systems. Nanomaterials, 2021, vol. 11, iss. 11, art. 2967. DOI: https://doi.org/10.3390/nano11112967

[29] Guo Y., Zhang X., Huang Z., et al. Quantum materials for spintronic applications. npj Spintronics, 2024, vol. 2, art. 36. DOI: https://doi.org/10.1038/s44306-024-00038-z