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Machine-learning-accelerated discovery of synthesizable high-temperature altermagnets with giant spin splitting

Materials Science 2026-05-28 v1

Abstract

Altermagnets offer a route to spin-polarized electronic states without macroscopic magnetization, because compensated magnetic order can generate momentum-dependent spin splitting through crystal-symmetry-controlled exchange fields. However, experimentally viable altermagnets combining large spin splitting, thermodynamic stability and high magnetic ordering temperatures remain scarce. Here, we develop a machine-learning-accelerated high-throughput framework to explore the tetragonal AB2_2C2_2D compounds. Screening 8640 variants identifies 1347 compensated antiferromagnetic candidates satisfying altermagnetic symmetry. An interpretable XGBoost model trained on first-principles spin-splitting data then isolates 34 low-hull-energy candidates,including four previously reported, with giant non-relativistic spin splittings exceeding 1.5 eV near the Fermi level. Detailed first-principles calculations of the representative RbMn2_2Te2_2O confirm a maximum spin splitting of \sim1.88 eV with dynamical stability and an estimated N\'eel temperature of \sim390 K. The giant splitting originates from symmetry-locked Mn-sublattice exchange fields amplified by directional Mn-d/Te-p hybridization. Furthermore, we uncover a profound soft-mode-driven structural transition associated with an interlayer dimensionality crossover in SrMn2_2Te2_2O, yet the unfolded electronic structure demonstrates that the altermagnetic spin splitting remains robust after lattice reconstruction. Hydrostatic pressure provides an additional tuning route, producing non-monotonic modulation of the spin-split Fermi surface governed by local coordination and orbital hybridization. These results establish tetragonal AB2_2C2_2D compounds as a tunable materials platform for stray-field-free spintronic devices and provide a general data-driven strategy for discovering robust giant-splitting altermagnets.

Keywords

Cite

@article{arxiv.2605.27888,
  title  = {Machine-learning-accelerated discovery of synthesizable high-temperature altermagnets with giant spin splitting},
  author = {Yi-Fei Jiang and Jia-Xuan Guo and Zhen Zhang and Xin-Wei Yi and Jing-Yang You},
  journal= {arXiv preprint arXiv:2605.27888},
  year   = {2026}
}

Comments

32 pages,6 figures