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Comparative study of magnetic exchange parameters and magnon dispersions in NiO and MnO from first principles

Flaviano José dos Santos1,2,3, Luca Binci4,5,6, Guido Menichetti7,8, Ruchika Mahajan9,10, Nicola Marzari1,6, and Iurii Timrov1,*

  • *Contact author: iurii.timrov@psi.ch
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Phys. Rev. B 113, 024427 – Published 22 January, 2026

DOI: https://doi.org/10.1103/gtxm-6vtg

Abstract

Spin-wave excitations are fundamental to understanding the behavior of magnetic materials and hold promise for future information and communication technologies. Yet, modeling these accurately in transition-metal compounds remains challenging, starting from the self-interaction errors affecting localized and partially filled d orbitals in density-functional theory (DFT) with (semi)local functionals. In this work, we compare three advanced first-principles approaches for computing magnetic exchange parameters and magnon dispersions in NiO and MnO, all based on a common DFT+U ground state with ab initio Hubbard U values obtained from density-functional perturbation theory. Two methods extract exchange parameters directly: one via total-energy differences using the four-state mapping (ΔE), and the other via the magnetic force theorem (MFT) using infinitesimal spin rotations. Magnon dispersions are then obtained from a Heisenberg Hamiltonian through linear spin-wave theory (LSWT). The third approach, time-dependent density-functional perturbation theory with U (TDDFPT+U), yields magnon dispersions directly from the dynamical spin susceptibility, with exchange parameters fitted a posteriori, for comparison, via LSWT. Our results show that TDDFPT+U and the Heisenberg model based on ΔE-derived parameters align well with experimental neutron scattering data, whereas the MFT-based approach shows larger discrepancies, possibly due to some inherent approximations and limitations of the particular implementation used. This study benchmarks the accuracy of state-of-the-art first-principles techniques for spin-wave modeling and contributes to advancing reliable computational tools for the study and design of magnetic materials.

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Phys. Rev. B 113, 024427– Published 22 January, 2026
  • Received 19 September 2025
  • Revised 11 December 2025
  • Accepted 5 January 2026
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