We report a comprehensive set of density functional theory calculations on the family of layered antiferromagnetic manganese pnictides (Ba, Ca, Sr)$\mathrm{ Mn}_2\mathrm{ (P, As, Sb)}_2$. We characterize all components to the linear magnetoelectric (ME) tensor $\alpha$ 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 $\alpha$ values exceeding those of the prototypical $\mathrm{ Cr}_2\mathrm{ O}_3$ (i.e. $\alpha \simeq$ 6.79 ps/m in $\mathrm{ BaMn}_2\mathrm{ As}_2$). We also identify a strong correlation with the computed ME susceptibility on pnictogen substitution in the trigonal subfamily albeit with weaker amplitudes ($\alpha \simeq$ 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.
Categories: cond-mat.mtrl-sci cond-mat.str-el