Benchmark for Ab Initio Prediction of Magnetic Structures Based on Cluster-Multipole Theory BENCHMARK for AB INITIO PREDICTION of ... HUEBSCH et al.

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 ±0.5μB. 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.