Pushing an Altermagnet to the Ultimate 2D Limit: Evidence of Symmetry Breaking in Monolayers of GdAlSi

Abstract: Altermagnets have emerged as a class of materials combining certain ferromagnetic properties with zero net magnetization. This combination is highly promising for spintronics, especially if a material can be brought to a nanoscale size. However, experimental studies of the 2D limit of altermagnets and evolution of their properties with thickness are lacking. Here, we study epitaxial films on silicon of the Weyl altermagnet GdAlSi ranging from more than a hundred unit cells to a single unit cell. The films are synthesized by molecular beam epitaxy and, expectedly, do not show any discernible net magnetic moments. Electron transport studies reveal a remarkable transformation of the electron state with the film thickness. Thick films exhibit negative longitudinal magnetoresistance associated with the chiral anomaly but do not demonstrate altermagnetic properties in electron transport due to symmetry restrictions. In ultrathin films, a spontaneous anomalous Hall effect manifests itself, indicating a non-relativistic spin splitting in the electronic structure. The transformation is associated with crystal symmetry breaking accompanying the 3D-to-2D crossover. The work highlights the role of dimensionality in altermagnetism and provides a platform for studies of altermagnets aiming at ultra-compact spintronics.