- Physical Review Journals
All JournalsPhysics Magazine

Physical Review B

Reuse & Permissions

It is not necessary to obtain permission to reuse this article or its components as it is available under the terms of the Creative Commons Attribution 4.0 International license. This license permits unrestricted use, distribution, and reproduction in any medium, provided attribution to the author(s) and the published article's title, journal citation, and DOI are maintained. Please note that some figures may have been included with permission from other third parties. It is your responsibility to obtain the proper permission from the rights holder directly for these figures.

Export citation

Export citation

Choose format for download:

Download Citation
  • Open Access

Polaron-mediated anisotropic exchange in two-dimensional magnets

Johanna P. Carbone1,*, Jakob Baumsteiger1,2,3, and Cesare Franchini1,3

  • 1Faculty of Physics and Center for Computational Materials Science, University of Vienna, Kolingasse 14-16, 1090 Vienna, Austria
  • 2Vienna Doctoral School in Physics, University of Vienna, ex Boltzmanngasse 5, 1090 Vienna, Austria
  • 3Department of Physics and Astronomy Augusto Righi, Alma Mater Studiorum, Università di Bologna, 40127 Bologna, Italy

  • *Contact author: johanna.paulina.carbone@univie.ac.at
PDF

Phys. Rev. B 113, 214428 – Published 10 June, 2026

DOI: https://doi.org/10.1103/rkgd-1qpj

Abstract

Two-dimensional (2D) magnets offer a rich platform for exploring emergent spin phenomena due to their unique and diverse magnetic properties. Beyond intrinsic magnetism, external manipulation—such as defect engineering, molecular adsorption, or charge doping—offers powerful routes to control their magnetic behavior. In this work, we demonstrate that localized electron polarons provide an effective means to modulate magnetism in 2D magnets. Using first-principles calculations, we investigate polaron formation in monolayer MnPS3 and compute the resulting changes in magnetic exchange interactions. Our results reveal that polarons can locally break magnetic symmetry and induce anisotropic exchange couplings, highlighting an alternative mechanism for tuning magnetic textures. This insight opens promising pathways for designing atomic-scale control of magnetism, with potential impact on spintronic technologies.

View figure in article

Physics Subject Headings (PhySH)

Article Text

References (53)

  1. M. Gibertini, M. Koperski, A. F. Morpurgo, and K. S. Novoselov, Magnetic 2D materials and heterostructures, Nat. Nanotechnol. 14, 408 (2019).
  2. S. Kumari, D. K. Pradhan, N. R. Pradhan, and P. D. Rack, Recent developments on 2D magnetic materials: Challenges and opportunities, Emergent Mater. 4, 827 (2021).
  3. Q. H. Wang, A. Bedoya-Pinto, M. Blei, A. H. Dismukes, A. Hamo, S. Jenkins, M. Koperski, Y. Liu, Q.-C. Sun, E. J. Telford, et al., The magnetic genome of two-dimensional van der Waals materials, ACS Nano 16, 6960 (2022).
  4. K. S. Novoselov, A. Mishchenko, A. Carvalho, and A. Castro Neto, 2D materials and van der Waals heterostructures, Science 353, aac9439 (2016).
  5. E. C. Ahn, 2D materials for spintronic devices, npj 2D Mater. Appl. 4, 17 (2020).
  6. S. Wei, X. Liao, C. Wang, J. Li, H. Zhang, Y.-J. Zeng, J. Linghu, H. Jin, and Y. Wei, Emerging intrinsic magnetism in two-dimensional materials: Theory and applications, 2D Mater. 8, 012005 (2021).
  7. D. Culcer, A. C. Keser, Y. Li, and G. Tkachov, Transport in two-dimensional topological materials: Recent developments in experiment and theory, 2D Mater. 7, 022007 (2020).
  8. K. Premasiri and X. P. Gao, Tuning spin–orbit coupling in 2D materials for spintronics: A topical review, J. Phys.: Condens. Matter 31, 193001 (2019).
  9. N. C. Frey, H. Kumar, B. Anasori, Y. Gogotsi, and V. B. Shenoy, Tuning noncollinear spin structure and anisotropy in ferromagnetic nitride MXenes, ACS Nano 12, 6319 (2018).
  10. S. Rahman, J. F. Torres, A. R. Khan, and Y. Lu, Recent developments in van der Waals antiferromagnetic 2D materials: Synthesis, characterization, and device implementation, ACS Nano 15, 17175 (2021).
  11. M. Hossain, B. Qin, B. Li, and X. Duan, Synthesis, characterization, properties and applications of two-dimensional magnetic materials, Nano Today 42, 101338 (2022).
  12. N. D. Mermin and H. Wagner, Absence of ferromagnetism or antiferromagnetism in one-or two-dimensional isotropic Heisenberg models, Phys. Rev. Lett. 17, 1133 (1966).
  13. H. Cheng, J. Zhou, M. Yang, L. Shen, J. Linghu, Q. Wu, P. Qian, and Y. P. Feng, Robust two-dimensional bipolar magnetic semiconductors by defect engineering, J. Mater. Chem. C 6, 8435 (2018).
  14. D. A. Mayoh, G. D. Wood, S. J. Holt, G. Beckett, E. J. Dekker, M. R. Lees, and G. Balakrishnan, Effects of Fe deficiency and Co substitution in polycrystalline and single crystals of Fe3GeTe2, Crystal Growth Design 21, 6786 (2021).
  15. Y. Zhao, L. Lin, Q. Zhou, Y. Li, S. Yuan, Q. Chen, S. Dong, and J. Wang, Surface vacancy-induced switchable electric polarization and enhanced ferromagnetism in monolayer metal trihalides, Nano Lett. 18, 2943 (2018).
  16. J. Kim, K.-W. Kim, B. Kim, C.-J. Kang, D. Shin, S.-H. Lee, B.-C. Min, and N. Park, Exploitable magnetic anisotropy of the two-dimensional magnet CrI3, Nano Lett. 20, 929 (2020).
  17. C. Song, W. Xiao, L. Li, Y. Lu, P. Jiang, C. Li, A. Chen, and Z. Zhong, Tunable band gap and enhanced ferromagnetism by surface adsorption in monolayer Cr2Ge2Te6, Phys. Rev. B 99, 214435 (2019).
  18. Y. Guo, S. Yuan, B. Wang, L. Shi, and J. Wang, Half-metallicity and enhanced ferromagnetism in Li-adsorbed ultrathin chromium triiodide, J. Mater. Chem. C 6, 5716 (2018).
  19. C. Tang, L. Zhang, and A. Du, Tunable magnetic anisotropy in 2D magnets via molecular adsorption, J. Mater. Chem. C 8, 14948 (2020).
  20. J. He, G. Ding, C. Zhong, S. Li, D. Li, and G. Zhang, Remarkably enhanced ferromagnetism in a super-exchange governed Cr2Ge2Te6 monolayer via molecular adsorption, J. Mater. Chem. C 7, 5084 (2019).
  21. M. Rassekh, J. He, S. F. Shayesteh, and J. J. Palacios, Remarkably enhanced Curie temperature in monolayer CrI3 by hydrogen and oxygen adsorption: A first-principles calculations, Comput. Mater. Sci. 183, 109820 (2020).
  22. K. Wang, K. Ren, Y. Cheng, S. Chen, and G. Zhang, The impacts of molecular adsorption on antiferromagnetic MnPS3 monolayers: Enhanced magnetic anisotropy and intralayer Dzyaloshinskii–Moriya interaction, Mater. Horiz. 9, 2384 (2022).
  23. M. Orozović, B. N. Šoškić, S. Picozzi, Ž. Šljivančanin, and S. Stavrić, Hole doping as an efficient route to increase the Curie temperature in monolayer CrI3, 2D Mater. 12, 045025 (2025).
  24. C. Franchini, M. Reticcioli, M. Setvin, and U. Diebold, Polarons in materials, Nat. Rev. Mater. 6, 560 (2021).
  25. D. Emin, Polarons (Cambridge University Press, Cambridge, UK, 2013).
  26. W. H. Sio and F. Giustino, Polarons in two-dimensional atomic crystals, Nat. Phys. 19, 629 (2023).
  27. H. Liu, A. Wang, P. Zhang, C. Ma, C. Chen, Z. Liu, Y.-Q. Zhang, B. Feng, P. Cheng, J. Zhao, et al., Atomic-scale manipulation of single-polaron in a two-dimensional semiconductor, Nat. Commun. 14, 3690 (2023).
  28. M. Cai, M.-P. Miao, Y. Liang, Z. Jiang, Z.-Y. Liu, W.-H. Zhang, X. Liao, L.-F. Zhu, D. West, S. Zhang, et al., Manipulating single excess electrons in monolayer transition metal dihalide, Nat. Commun. 14, 3691 (2023).
  29. L. Yao, A. Wang, Q. Zheng, and J. Zhao, Small polaron dynamics in a two-dimensional magnetic material, Phys. Rev. B 110, 054305 (2024).
  30. H. Rho, C. S. Snow, S. L. Cooper, Z. Fisk, A. Comment, and J.-P. Ansermet, Evolution of magnetic polarons and spin-carrier interactions through the metal-insulator transition in Eu1−xGdxO, Phys. Rev. Lett. 88, 127401 (2002).
  31. L. Celiberti, D. Fiore Mosca, G. Allodi, L. V. Pourovskii, A. Tassetti, P. C. Forino, R. Cong, E. Garcia, P. M. Tran, R. De Renzi, et al., Spin-orbital Jahn-Teller bipolarons, Nat. Commun. 15, 2429 (2024).
  32. J. Redondo, M. Reticcioli, V. Gabriel, D. Wrana, F. Ellinger, M. Riva, G. Franceschi, E. Rheinfrank, I. Sokolović, Z. Jakub, et al., Real-space investigation of polarons in hematite Fe2O3, Sci. Adv. 10, eadp7833 (2024).
  33. D. F. Mosca, L. Celiberti, L. V. Pourovskii, and C. Franchini, Polaron-driven switching of octupolar order in doped 5d2 double perovskite, arXiv:2603.18155.
  34. S. N. Neal, H.-S. Kim, K. A. Smith, A. V. Haglund, D. G. Mandrus, H. A. Bechtel, G. L. Carr, K. Haule, D. Vanderbilt, and J. L. Musfeldt, Near-field infrared spectroscopy of monolayer MnPS3, Phys. Rev. B 100, 075428 (2019).
  35. R.-C. Xiao, D.-F. Shao, Y.-H. Li, and H. Jiang, Spin photogalvanic effect in two-dimensional collinear antiferromagnets, npj Quantum Mater. 6, 35 (2021).
  36. C. Liu, W. Ren, and S. Picozzi, Spin-chirality-driven multiferroicity in van der Waals monolayers, Phys. Rev. Lett. 132, 086802 (2024).
  37. B. H. Rimmler, B. Pal, and S. S. Parkin, Non-collinear antiferromagnetic spintronics, Nat. Rev. Mater. 10, 109 (2025).
  38. P.-X. Qin, H. Yan, X.-N. Wang, Z.-X. Feng, H.-X. Guo, X.-R. Zhou, H.-J. Wu, X. Zhang, Z.-G.-G. Leng, H.-Y. Chen, et al., Noncollinear spintronics and electric-field control: A review, Rare Metals 39, 95 (2020).
  39. T. Jungwirth, J. Sinova, A. Manchon, X. Marti, J. Wunderlich, and C. Felser, The multiple directions of antiferromagnetic spintronics, Nat. Phys. 14, 200 (2018).
  40. Y. Gao, X. Jiang, Z. Qiu, and J. Zhao, Photoexcitation induced magnetic phase transition and spin dynamics in antiferromagnetic MnPS3 monolayer, npj Comput. Mater. 9, 107 (2023).
  41. R. Samal, G. Sanyal, B. Chakraborty, and C. S. Rout, Two-dimensional transition metal phosphorous trichalcogenides (MPX3): A review on emerging trends, current state and future perspectives, J. Mater. Chem. A 9, 2560 (2021).
  42. J. Yang, Y. Zhou, Q. Guo, Y. Dedkov, and E. Voloshina, Electronic, magnetic and optical properties of MnPX3 (X= S, Se) monolayers with and without chalcogen defects: A first-principles study, RSC Adv. 10, 851 (2020).
  43. G. Kresse and J. Furthmüller, Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set, Phys. Rev. B 54, 11169 (1996).
  44. J. P. Perdew, K. Burke, and M. Ernzerhof, Generalized gradient approximation made simple, Phys. Rev. Lett. 77, 3865 (1996).
  45. S. L. Dudarev, G. A. Botton, S. Y. Savrasov, C. J. Humphreys, and A. P. Sutton, Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study, Phys. Rev. B 57, 1505 (1998).
  46. S. Picozzi, Spin–orbit coupling in quantum materials: Emergent phenomena, their modelling and examples from two-dimensional magnets, Riv. Nuovo Cimento 47, 609 (2024).
  47. X. Li, H. Yu, F. Lou, J. Feng, M.-H. Whangbo, and H. Xiang, Spin Hamiltonians in magnets: Theories and computations, Molecules 26, 803 (2021).
  48. H. J. Xiang, E. J. Kan, S.-H. Wei, M.-H. Whangbo, and X. G. Gong, Predicting the spin-lattice order of frustrated systems from first principles, Phys. Rev. B 84, 224429 (2011).
  49. M. Reticcioli, U. Diebold, G. Kresse, and C. Franchini, Small polarons in transition metal oxides, in Handbook of Materials Modeling (Springer, Cham, 2020), pp. 1–39.
  50. K. Momma and F. Izumi, VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data, J. Appl. Crystallogr. 44, 1272 (2011).
  51. T. Olsen, Magnetic anisotropy and exchange interactions of two-dimensional FePS3, NiPS3 and MnPS3 from first principles calculations, J. Phys. D 54, 314001 (2021).
  52. R. Basnet, K. M. Kotur, M. Rybak, C. Stephenson, S. Bishop, C. Autieri, M. Birowska, and J. Hu, Controlling magnetic exchange and anisotropy by nonmagnetic ligand substitution in layered MPX3 (M = Ni, Mn; X = S, Se), Phys. Rev. Res. 4, 023256 (2022).
  53. J.-T. Yang, C.-J. Xu, H.-J. Wang, Q. Min, S.-J. Luo, Y.-C. Xiong, W. Ren, and C. Jing, Stable antiferromagnetic property and tunable electronic structure of two-dimensional MnPX3 (X = S and Se) from pristine structure to Janus phase, J. Phys.: Condens. Matter 35, 395501 (2023).

Outline

Information

Phys. Rev. B 113, 214428– Published 10 June, 2026
  • Received 4 November 2025
  • Revised 6 March 2026
  • Accepted 13 May 2026
Crossmark - Check for updates button
Creative Commons Logo

Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.

Published by the American Physical Society

Sign In to Your Journals Account

Filter

Filter

Article Lookup

Enter a citation