General spin models from noncollinear spin density functional theory and spin-cluster expansion

Abstract

We present a data-efficient framework for constructing general classical spin Hamiltonians by combining the spin-cluster expansion (SCE) with fully self-consistent noncollinear spin density functional theory (DFT). The key idea is to fit the SCE model to magnetic torques rather than to total energies. Because torques are site-resolved vectors, each spin configuration provides many informative regression targets, improving conditioning and substantially reducing the number of required DFT calculations, especially for large supercells. Applied to the B20-type chiral magnets ${\rm Mn}_{1-x}{\rm Fe}_{x}{\rm Ge}$ and ${\rm Fe}_{1-y}{\rm Co}_{y}{\rm Ge}$, the resulting SCE models determine full pairwise exchange tensors -- including isotropic exchange, symmetric anisotropic exchange, and the Dzyaloshinskii--Moriya interaction -- and predict the helical spin period via a micromagnetic mapping. The composition trends and the divergence of the period at the chirality sign-change point are well reproduced, in agreement with experiment. Moreover, the systematic nature of SCE enables controlled assessment of interaction order: as the training spin configurations become more disordered, the lowest-order model loses torque accuracy, whereas including higher-order interactions restores predictive power. These advances enable near-DFT-accurate spin models for finite-temperature magnetism and complex spin textures at modest computational cost, providing an extensible route to quantitative first-principles parameterization and predictive materials design. An open-source implementation is available as a Julia package, \textit{Magesty.jl}.