Complex Magnetic Interactions in Geometrically Frustrated TbOF

We have identified TbOF as a unique frustrated and mixed-anion lattice, hosting unconventional magnetism. By means of magnetization, specific heat, and neutron diffraction measurements down to 90 mK, as well as DFT calculations, we present a comprehensive study of the magnetic and structural properties of TbOF. We show that at 9.7 K, TbOF undergoes a structural phase transition accompanied by short-range magnetic correlations, in contrast to previously proposed long-range antiferromagnetic order. At lower temperatures, we observe two magnetic ordering transitions, consisting of incommensurate spin density waves and antiferromagnetic and ferromagnetic correlations. Furthermore, we observe metastable and hysteresis behavior below 2.0 K, highlighting the richness of complex magnetic interactions in TbOF. These results uniquely clarify the magnetic phase diagram of TbOF and highlight the intricate interplay between structure and magnetism in rare-earth oxyfluorides.