Benchmark for <i>Ab Initio</i> Prediction of Magnetic Structures Based on Cluster-Multipole Theory
M.-T. Huebsch, T. Nomoto, M.-T. Suzuki, R. Arita
Abstract
The cluster-multipole (CMP) expansion for magnetic structures provides a scheme to systematically generate candidate magnetic structures specifically including noncollinear magnetic configurations adapted to the crystal symmetry of a given material. A comparison with the experimental data collected on MAGNDATA shows that the most stable magnetic configurations in nature are linear combinations of only few CMPs. Furthermore, a high-throughput calculation for all candidate magnetic structures is performed in the framework of spin-density functional theory (SDFT). We benchmark the predictive power of CMP SDFT with 2935 calculations, which show that (i) the CMP expansion administers an exhaustive list of candidate magnetic structures, (ii) CMP SDFT can narrow down the possible magnetic configurations to a handful of computed configurations, and (iii) SDFT reproduces the experimental magnetic configurations with an accuracy of AE0.5 B . For a subset the impact of on-site Coulomb repulsion U is investigated by means of 1545 CMP SDFT U calculations revealing no further improvement on the predictive power.