We report a comprehensive set of density functional theory calculations on the family of layered antiferromagnetic manganese pnictides (Ba, Ca, Sr)Mn2(P,As,Sb)2. We characterize all components to the linear magnetoelectric (ME) tensor α which are parsed into their contributions from spin and orbital moments for both lattice-mediated and their clamped-ion electronic analogs. Our main results show that the orbital magnetization components cannot be neglected in these systems. The ME response is dominated by electronic effects with total α values exceeding those of the prototypical Cr2O3 (i.e. α≃ 6.79 ps/m in BaMn2As2). We also identify a strong correlation with the computed ME susceptibility on pnictogen substitution in the trigonal subfamily albeit with weaker amplitudes (α≃ 0.2-1.7 ps/m). Additionally, we provide the dependence of these predictions on the Hubbard +U correction, at the level of the local density approximation, which show large variations on the calculated ME coefficients in the tetragonal compounds highlighting the role of strong correlation in these compounds.
@article{arxiv.2403.15222,
title = {Linear magnetoelectricity in the Zintl phase pnictides (Ba, Ca, Sr)$\mathrm{Mn}_2\mathrm{(P, As, Sb)}_2$ from first principles calculations},
author = {John Mangeri and Martin Ovesen and Thomas Olsen},
journal= {arXiv preprint arXiv:2403.15222},
year = {2024}
}