Anisotropy of antiferromagnetic 180 degrees domains in LiCoPO4 and LiNiPO4.

Unexpected three-dimensional distributions of antiferromagnetic 180 degrees domains are observed in LiCoPO4 and LiNiPO4 by optical second harmonic generation. Domains in LiCoPO4 are isotropic in spite of the quasi-two-dimensional magnetic structure whereas domains in LiNiPO4 are distinctly anisotropic, but in contrast to the anisotropy of the magnetic structure. The diversity reveals a potential for fine-tuning magnetic properties determined by the distribution of domains or domain walls and the urgent need for an improved understanding of spatial correlations in antiferromagnets.