Antiferromagnetic Order of the Co²⁺ High-Spin State with a Large Orbital Angular Momentum in La_1.5Ca_0.5CoO₄

Abstract

The antiferromagnetic insulator La1.5Ca0.5CoO4 has been investigated by Co L2,3-edge and O K-edge X-ray absorption spectroscopy (XAS) measurements and Co L2,3-edge resonant soft X-ray magnetic scattering (RXMS) measurement to determine the Co electronic structures associated with magnetic ordering. Co L2,3-edge linear-dichroic XAS shows that Co2+ takes a high-spin (HS) state and Co3+ takes a low-spin (LS) state. Using Co L2,3-edge RXMS, we directly determined that an antiferromagnetic order is formed with a HS state of Co2+ ions. Moreover, the spin and orbital angular momenta of the Co2+ HS state are quantitatively estimated to be 1.1 ± 0.1 and 1.0 ± 0.1, respectively, and to align parallel in the ab plane by utilizing the cluster model calculation. The large orbital angular momentum of the Co2+ HS state originates from the small D4h-symmetry crystal field splitting of t2g levels, which is comparable with the spin–orbit coupling constant of the Co 3d orbital.