Temperature-Dependent Magnetoelectric Effect from First Principles

We show that nonrelativistic exchange interactions and spin fluctuations can give rise to a linear magnetoelectric effect in collinear antiferromagnets at elevated temperatures that can exceed relativistic magnetoelectric responses by more than 1 order of magnitude. We show how symmetry arguments, ab initio methods, and Monte Carlo simulations can be combined to calculate temperature-dependent magnetoelectric susceptibilities entirely from first principles. The application of our method to Cr2O3 gives quantitative agreement with experiment.