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We derive a quantum-mechanical formula of the orbital magnetic quadrupole moment (MQM) in periodic systems by using the gauge-covariant gradient expansion. This formula is valid for insulators and metals at zero and finite temperature. We also prove a direct relation between the MQM and magnetoelectric (ME) susceptibility for insulators at zero temperature. It indicates that the MQM is a microscopic origin of the ME effect. Using the formula, we quantitatively estimate these quantities for room-temperature antiferromagnetic semiconductors BaMn$_2$As$_2$ and CeMn$_2$Ge$_{2 - x}$Si$_x$. We find that the orbital contribution to the ME susceptibility is comparable with or even dominant over the spin contribution.
The theoretical treatment of homogeneous static magnetic fields in periodic systems is challenging, as the corresponding vector potential breaks the translational invariance of the Hamiltonian. Based on density operators and perturbation theory, we p
A general formula for the orbital magnetic moment of interacting electrons in solids is derived using the many-electron Green function method. The formula factorizes into two parts, a part that contains the information about the one-particle band str
We use symmetry analysis and first principles calculations to show that the linear magnetoelectric effect can originate from the response of orbital magnetic moments to the polar distortions induced by an applied electric field. Using LiFePO4 as a mo
We report electronic structure calculations of an iron impurity in gold host. The spin, orbital and dipole magnetic moments were investigated using the LDA+$U$ correlated band theory. We show that the {em around-mean-field}-LDA+$U$ reproduces the XMC
Titanium disulfide TiS$_2$, which is a member of the layered transition-metal dichalcogenides with the 1T-CdI$_2$-type crystal structure, is known to exhibit a wide variety of magnetism through intercalating various kinds of transition-metal atoms of