Two-dimensional van der Waals (vdW) magnets offer unprecedented opportunities to control magnetism at the atomic scale. Through charge carrier doping-realized by electrostatic gating, intercalation/adsorption, or interfacial charge transfer-one can efficiently tune exchange interactions and spin-orbit-induced effects in these systems. In this work, through a multi-scale theoretical framework combining density functional theory, spin Hamiltonian modeling, and Wannierfunction analysis, we choose monolayer CrI3 to unravel how carrier doping affects the isotropic as well as anisotropic exchange interactions in this prototypical vdW ferromagnet. The remarkable efficiency of hole doping in enhancing ferromagnetic exchange and magnetic anisotropy found in our study was explained through orbital-resolved analysis. Crucially, we demonstrated that unlike the undoped system-where isotropic exchange interactions govern magnetic long-range order- the hole-doped CrI3 exhibits anisotropic terms compa...rable in magnitude to isotropic ones. In particular, the magnetic anisotropy energy increases from 0.65 meV in undoped to 4.43 meV in strongly hole-doped CrI3, with the second-neighbor Dzyaloshinskii-Moriya interaction increasing from 0.12 meV to 2.01 meV. Finally, we show that a high concentration of holes can increase the Curie temperature from 56 K all the way up to 228 K. This work advances our understanding of doping-controlled magnetism in semiconducting 2D materials, demonstrating how anisotropy engineering can stabilize high-temperature magnetic order.
TY - JOUR
AU - Orozović, Marko
AU - Šoškić, Božidar N.
AU - Picozzi, Silvia
AU - Šljivančanin, Željko
AU - Stavrić, Srđan
PY - 2025
UR - https://vinar.vin.bg.ac.rs/handle/123456789/16107
AB - Two-dimensional van der Waals (vdW) magnets offer unprecedented opportunities to control magnetism at the atomic scale. Through charge carrier doping-realized by electrostatic gating, intercalation/adsorption, or interfacial charge transfer-one can efficiently tune exchange interactions and spin-orbit-induced effects in these systems. In this work, through a multi-scale theoretical framework combining density functional theory, spin Hamiltonian modeling, and Wannierfunction analysis, we choose monolayer CrI3 to unravel how carrier doping affects the isotropic as well as anisotropic exchange interactions in this prototypical vdW ferromagnet. The remarkable efficiency of hole doping in enhancing ferromagnetic exchange and magnetic anisotropy found in our study was explained through orbital-resolved analysis. Crucially, we demonstrated that unlike the undoped system-where isotropic exchange interactions govern magnetic long-range order- the hole-doped CrI3 exhibits anisotropic terms comparable in magnitude to isotropic ones. In particular, the magnetic anisotropy energy increases from 0.65 meV in undoped to 4.43 meV in strongly hole-doped CrI3, with the second-neighbor Dzyaloshinskii-Moriya interaction increasing from 0.12 meV to 2.01 meV. Finally, we show that a high concentration of holes can increase the Curie temperature from 56 K all the way up to 228 K. This work advances our understanding of doping-controlled magnetism in semiconducting 2D materials, demonstrating how anisotropy engineering can stabilize high-temperature magnetic order.
T2 - 2d Materials
T1 - Hole doping as an efficient route to increase the Curie temperature in monolayer CrI3
VL - 12
IS - 4
SP - 45025
DO - 10.1088/2053-1583/ae1512
ER -
@article{
author = "Orozović, Marko and Šoškić, Božidar N. and Picozzi, Silvia and Šljivančanin, Željko and Stavrić, Srđan",
year = "2025",
abstract = "Two-dimensional van der Waals (vdW) magnets offer unprecedented opportunities to control magnetism at the atomic scale. Through charge carrier doping-realized by electrostatic gating, intercalation/adsorption, or interfacial charge transfer-one can efficiently tune exchange interactions and spin-orbit-induced effects in these systems. In this work, through a multi-scale theoretical framework combining density functional theory, spin Hamiltonian modeling, and Wannierfunction analysis, we choose monolayer CrI3 to unravel how carrier doping affects the isotropic as well as anisotropic exchange interactions in this prototypical vdW ferromagnet. The remarkable efficiency of hole doping in enhancing ferromagnetic exchange and magnetic anisotropy found in our study was explained through orbital-resolved analysis. Crucially, we demonstrated that unlike the undoped system-where isotropic exchange interactions govern magnetic long-range order- the hole-doped CrI3 exhibits anisotropic terms comparable in magnitude to isotropic ones. In particular, the magnetic anisotropy energy increases from 0.65 meV in undoped to 4.43 meV in strongly hole-doped CrI3, with the second-neighbor Dzyaloshinskii-Moriya interaction increasing from 0.12 meV to 2.01 meV. Finally, we show that a high concentration of holes can increase the Curie temperature from 56 K all the way up to 228 K. This work advances our understanding of doping-controlled magnetism in semiconducting 2D materials, demonstrating how anisotropy engineering can stabilize high-temperature magnetic order.",
journal = "2d Materials",
title = "Hole doping as an efficient route to increase the Curie temperature in monolayer CrI3",
volume = "12",
number = "4",
pages = "45025",
doi = "10.1088/2053-1583/ae1512"
}
Orozović, M., Šoškić, B. N., Picozzi, S., Šljivančanin, Ž.,& Stavrić, S.. (2025). Hole doping as an efficient route to increase the Curie temperature in monolayer CrI3. in 2d Materials, 12(4), 45025.
https://doi.org/10.1088/2053-1583/ae1512
Orozović M, Šoškić BN, Picozzi S, Šljivančanin Ž, Stavrić S. Hole doping as an efficient route to increase the Curie temperature in monolayer CrI3. in 2d Materials. 2025;12(4):45025.
doi:10.1088/2053-1583/ae1512 .
Orozović, Marko, Šoškić, Božidar N., Picozzi, Silvia, Šljivančanin, Željko, Stavrić, Srđan, "Hole doping as an efficient route to increase the Curie temperature in monolayer CrI3" in 2d Materials, 12, no. 4 (2025):45025,
https://doi.org/10.1088/2053-1583/ae1512 . .
