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We present a Wannier-based method to calculate the Chern-Simons orbitalmagnetoelectric coupling in the framework of first-principlesdensity-functional theory. In view of recent developments in connection withstrong Z2 topological insulators, we anticipate that the Chern-Simonscontribution to the magnetoelectric coupling could, in special cases, be aslarge or larger than the total magnetoelectric coupling in knownmagnetoelectrics like Cr2O3. The results of our calculations for the ordinarymagnetoelectrics Cr2O3, BiFeO3 and GdAlO3 confirm that the Chern-Simonscontribution is quite small in these cases. On the other hand, we show that ifthe spatial inversion and time-reversal symmetries of the Z2 topologicalinsulator Bi2Se3 are broken by hand, large induced changes appear in theChern-Simons magnetoelectric coupling.

Chern-Simons orbital magnetoelectric coupling in generic insulators