Dynamical response of noncollinear spin systems at constrained magnetic moments

Fuente: arXiv
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Main Authors: Royo, Miquel, Stengel, Massimiliano
Format: Preprint
Published: 2025
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author Royo, Miquel
Stengel, Massimiliano
author_facet Royo, Miquel
Stengel, Massimiliano
contents Noncollinear magnets are notoriously difficult to describe within first-principles approaches based on density-functional theory (DFT) because of the presence of low-lying spin excitations. At the level of ground-state calculations, several methods exist to constrain the magnetic moments to a predetermined configuration, and thereby accelerate convergence towards self-consistency. Their use in a perturbative context, however, remains very limited. Here we present a general methodological framework to achieve parametric control over the local spin moments at the linear-response level. Our strategy builds on the concept of Legendre transform to switch between various flavors of magnetic functionals, and to relate their second derivatives via simple linear-algebra operations. Thereby, we can address an arbitrary response function at the time-dependent DFT level of theory with optimal accuracy and minimal computational effort. In the low frequency limit, we identify the leading correction to the existing adiabatic formulation of the problem [S. Ren \emph{et al.}, Phys. Rev. X {\bf 14}, 011041 (2024)], consisting in a renormalization of the phonon and magnon masses due to electron inertia. As a demonstration, we apply our methodology to the THz optical response of bulk CrI$_3$ and Cr$_2$O$_3$, where we identify contributions from hybrid (electro)magnons with mixed spin-lattice character.
format Preprint
id arxiv_https___arxiv_org_abs_2501_10188
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Dynamical response of noncollinear spin systems at constrained magnetic moments
Royo, Miquel
Stengel, Massimiliano
Materials Science
Mesoscale and Nanoscale Physics
Noncollinear magnets are notoriously difficult to describe within first-principles approaches based on density-functional theory (DFT) because of the presence of low-lying spin excitations. At the level of ground-state calculations, several methods exist to constrain the magnetic moments to a predetermined configuration, and thereby accelerate convergence towards self-consistency. Their use in a perturbative context, however, remains very limited. Here we present a general methodological framework to achieve parametric control over the local spin moments at the linear-response level. Our strategy builds on the concept of Legendre transform to switch between various flavors of magnetic functionals, and to relate their second derivatives via simple linear-algebra operations. Thereby, we can address an arbitrary response function at the time-dependent DFT level of theory with optimal accuracy and minimal computational effort. In the low frequency limit, we identify the leading correction to the existing adiabatic formulation of the problem [S. Ren \emph{et al.}, Phys. Rev. X {\bf 14}, 011041 (2024)], consisting in a renormalization of the phonon and magnon masses due to electron inertia. As a demonstration, we apply our methodology to the THz optical response of bulk CrI$_3$ and Cr$_2$O$_3$, where we identify contributions from hybrid (electro)magnons with mixed spin-lattice character.
title Dynamical response of noncollinear spin systems at constrained magnetic moments
topic Materials Science
Mesoscale and Nanoscale Physics
url https://arxiv.org/abs/2501.10188