Formation of a simple cubic antiferromagnet through charge ordering in a double Dirac material

While the topological classification of matter has resulted in the prediction and detection of unique topological phases in both insulators and metals, materials that support an interplay between topology and interactions are particularly interesting. We report the discovery that the topologically non-trivial cubic double Dirac metal EuPd3S4 undergoes long-range charge ordering at TCO = 340 K wherein Eu ions on a body-centered-cubic lattice divide into interpenetrating simple cubic lattices, one occupied by magnetic Eu2+ the other by non-magnetic Eu3+. The reduced symmetry transmutes the 8-fold double Dirac states into 4-fold Dirac states and leads to the formation of an isotropic simple cubic Heisenberg antiferromagnet (AFM) that subsequently develops G-type AFM order at TN = 2.85(6) K. While time reversal symmetry is broken at this second order phase transition, its combination with the nearest neighbor lattice translation forms a non-symmorphic symmetry operation that preserves the 4-fold Dirac point. Application of a magnetic field at low temperatures yields a spin flop transition followed by a fully magnetized charge ordered state. Our work demonstrates how the collective phenomena of charge and spin ordering in EuPd3S4 modify electronic topology and provides a full experimental view of the field-temperature phase diagram of the simple cubic Heisenberg antiferromagnet.