Orbital Magnetization in Extended Systems

While the orbital magnetic dipole moment of any finite sample is well‐defined, it becomes ill‐defined in the thermodynamic limit as a result of the unboundedness of the position operator. Effects due to surface currents and to bulk magnetization are not easily disentangled. The corresponding electrical problem, where surface charges and bulk polarization appear as entangled, was solved about a decade ago by the modern theory of polarization, based on a Berry phase. We follow a similar path here, making progress toward a bulk expression for the orbital magnetization in an insulator represented by a lattice‐periodic Hamiltonian with broken time‐reversal symmetry. We therefore limit ourselves to the case where the macroscopic (i.e. cell‐averaged) magnetic field vanishes. We derive an expression for the contribution to the magnetization arising from the circulating currents internal to the bulk Wannier functions, and then transform to obtain a Brillouin zone integral involving the occupied Bloch orbitals. A version suitable for practical implementation in discretized reciprocal space is also derived, and the gauge invariance of both versions is explicitly shown. However, tests on a tight‐binding model indicate the presence of additional edge currents, and it remains to be determined whether these can be related to the bulk band structure.