Magnetism of pseudospin-1/2 pyrochlore antiferromagnet Na₃Co(CO₃)₂Cl

Pyrochlore magnets have attracted interest as systems for realizing critical phenomena, rich magnetic structures, associated topological band structures, and nontrivial quantum phases. Na₃Co(CO₃)₂Cl is a pseudospin-1/2 antiferromagnet in which the Co²⁺ions form a pyrochlore network. Its structural and magnetic properties were investigated using magnetization, heat capacity, ESR, single-crystal x-ray diffraction, powder neutron diffraction and powder inelastic neutron scattering. Magnetization and heat capacity measurements indicated a ground-state doublet, which is regarded as pseudospin 1/2, dominated the magnetic properties at low temperatures, with a magnetic exchange of 9.6 K. As the temperature decreases, a magnetic transition is observed at 1.6 K, which is confirmed to be an all-in-all-out magnetic order. The crystal field excitations observed by inelastic neutron scattering experiments indicated the Ising nature of the ground-state doublet. This thorough study revealed that Na₃Co(CO₃)₂Cl can be regarded as a pseudospin-1/2 pyrochlore lattice antiferromagnet with dominant Ising-type interactions.