Exploring noncollinear magnetic energy landscapes with Bayesian optimization

Abstract

The investigation of magnetic energy landscapes and the search for ground states of magnetic materials using ab initio methods like density functional theory (DFT) is a challenging task. Complex interactions, such as superexchange and spin–orbit coupling, make these calculations computationally expensive and often lead to non-trivial energy landscapes. Consequently, a comprehensive and systematic investigation of large magnetic configuration spaces is often impractical. We approach this problem by utilizing Bayesian optimization, an active machine learning scheme that has proven to be efficient in modeling unknown functions and finding global minima. Using this approach we can obtain the magnetic contribution to the energy as a function of one or more spin canting angles with relatively small numbers of DFT calculations. To assess the capabilities and the efficiency of the approach we investigate the noncollinear magnetic energy landscapes of selected materials containing 3d, 5d and 5f magnetic ions: Ba₃MnNb₂O₉, LaMn₂Si₂, β-MnO₂, Sr₂IrO₄, UO₂, Ba₂NaOsO₆ and kagome RhMn₃. By comparing our results to previous ab initio studies that followed more conventional approaches, we observe significant improvements in efficiency.