Magnons from time-dependent density-functional perturbation theory and nonempirical Hubbard functionals

DOI

Spin excitations play a fundamental role in understanding magnetic properties of materials, and have significant technological implications for magnonic devices. However, accurately modeling these in transition-metal and rare-earth compounds remains a formidable challenge. Here, we present a fully first-principles approach for calculating spin-wave spectra based on time-dependent (TD) density-functional perturbation theory (DFPT), using nonempirical Hubbard functionals. This approach is implemented in a general noncollinear formulation, enabling the study of magnons in both collinear and noncollinear magnetic systems. Unlike methods that rely on empirical Hubbard U parameters to describe the ground state, and Heisenberg Hamiltonians for describing magnetic excitations, the methodology developed here probes directly the dynamical spin susceptibility (efficiently evaluated with TDDFPT throught the Liouville-Lanczos approach), and treats the linear variation of the Hubbard augmentation (in itself calculated non-empirically) in full at a self-consistent level. Furthermore, the method satisfies the Goldstone condition without requiring empirical rescaling of the exchange-correlation kernel or explicit enforcement of sum rules, in contrast to existing state-of-the-art techniques. We benchmark the novel computational scheme on prototypical transition-metal monoxides NiO and MnO, showing remarkable agreement with experiments and highlighting the fundamental role of these newly implemented Hubbard corrections. The method holds great promise for describing collective spin excitations in complex materials containing localized electronic states.

Identifier
DOI https://doi.org/10.24435/materialscloud:x3-z3
Related Identifier https://doi.org/10.48550/arXiv.2409.19504
Related Identifier https://doi.org/10.1038/s41524-025-01570-0
Related Identifier https://archive.materialscloud.org/communities/mcarchive
Related Identifier https://doi.org/10.24435/materialscloud:7c-6j
Metadata Access https://archive.materialscloud.org/oai2d?verb=GetRecord&metadataPrefix=oai_dc&identifier=oai:materialscloud.org:2601
Provenance
Creator Binci, Luca; Marzari, Nicola; Timrov, Iurii
Publisher Materials Cloud
Contributor Binci, Luca; Marzari, Nicola; Timrov, Iurii
Publication Year 2025
Rights info:eu-repo/semantics/openAccess; Creative Commons Attribution 4.0 International; https://creativecommons.org/licenses/by/4.0/legalcode
OpenAccess true
Contact archive(at)materialscloud.org
Representation
Language English
Resource Type info:eu-repo/semantics/other
Format text/markdown; application/zip
Discipline Materials Science and Engineering