Abstract
We report time-of-flight neutron spectroscopy and neutron and x-ray diffraction studies of the 5d2 double perovskite magnets, Ba2MOsO6 (M=Zn,Mg,Ca). These materials host antiferromagnetically coupled 5d2 Os6+ ions decorating a face-centered cubic (fcc) lattice and are found to remain cubic down to the lowest temperatures. They all exhibit thermodynamic anomalies consistent with a single phase transition at a temperature T∗, and a gapped magnetic excitation spectrum with spectral weight concentrated at wave vectors typical of type-I antiferromagnetic orders. However, while muon spin resonance experiments show clear evidence for time-reversal symmetry breaking below T∗, we observe no corresponding magnetic Bragg scattering signal. These results are shown to be consistent with ferro-octupolar symmetry breaking below T∗, and are discussed in the context of other 5d double perovskite magnets and theories of exotic orders driven by multipolar interactions.
