First-principles theory of magnetically induced ferroelectricity in TbMnO3

We study the polarization induced via spin-orbit interaction by a magnetic cycloidal order in orthorhombic TbMnO3 using first-principle methods. The case of magnetic spiral lying in the b-c plane is analyzed, in which the pure electronic contribution to the polarization is shown to be small. We focus our attention on the lattice-mediated contribution, and study it's dependence on the Coulomb interaction parameter U in the LDA+U method and on the wave-vector of the spin spiral. The role of the spin-orbit interaction on different sites is also analyzed.Comment: 4 pages, 2 figures, submitted to EPJ B (MEIPIC6 proceedings

First-principles DFT+GW study of oxygen vacancies in rutile TiO2

We perform first-principles calculations of the quasiparticle defect states, charge transition levels, and formation energies of oxygen vacancies in rutile titanium dioxide. The calculations are done within the recently developed combined DFT+GW formalism, including the necessary electrostatic corrections for the supercells with charged defects. We find the oxygen vacancy to be a negative U defect, where U is the defect electron addition energy. For the values of Fermi level below 2.8 eV (relative to the valence band maximum) we find the +2 charge state of the vacancy to be the most stable, while above 2.8 eV we find that the neutral charge state is the most stable

Orbital magnetoelectric coupling at finite electric field

We extend the band theory of linear orbital magnetoelectric coupling to treat crystals under finite electric fields. Previous work established that the orbital magnetoelectric response of a generic insulator at zero field comprises three contributions that were denoted as local circulation, itinerant circulation, and Chern-Simons. We find that the expression for each of them is modified by the presence of a dc electric field. Remarkably, the sum of the three correction terms vanishes, so that the total coupling is still given by the same formula as at zero field. This conclusion is confirmed by numerical tests on a tight-binding model, for which we calculate the field-induced change in the linear magnetoelectric coefficient.Comment: 4 pages, 2 figure

Full magnetoelectric response of Cr2O3 from first principles

The linear magnetoelectric response of Cr2O3 at zero temperature is calculated from first principles by tracking the change in magnetization under a macroscopic electric field. Both the spin and the orbital contributions to the induced magnetization are computed, and in each case the response is decomposed into lattice and electronic parts. We find that the transverse response is dominated by the spin-lattice and spin-electronic contributions, whose calculated values are consistent with static and optical magnetoelectric measurements. In the case of the longitudinal response, orbital contributions dominate over spin contributions, but the net calculated longitudinal response remains much smaller than the experimentally measured one at low temperatures. We also discuss the absolute sign of the magnetoelectric coupling in the two time-reversed magnetic domains of Cr2O3.Comment: 7 pages, 1 figur

Chern-Simons orbital magnetoelectric coupling in generic insulators

We present a Wannier-based method to calculate the Chern-Simons orbital magnetoelectric coupling in the framework of first-principles density-functional theory. In view of recent developments in connection with strong Z2 topological insulators, we anticipate that the Chern-Simons contribution to the magnetoelectric coupling could, in special cases, be as large or larger than the total magnetoelectric coupling in known magnetoelectrics like Cr2O3. The results of our calculations for the ordinary magnetoelectrics Cr2O3, BiFeO3 and GdAlO3 confirm that the Chern-Simons contribution is quite small in these cases. On the other hand, we show that if the spatial inversion and time-reversal symmetries of the Z2 topological insulator Bi2Se3 are broken by hand, large induced changes appear in the Chern-Simons magnetoelectric coupling.Comment: 13 pages, 8 figures, 1 tabl

Dependence of electronic polarization on octahedral rotations in TbMnO3 from first principles

The electronic contribution to the magnetically induced polarization in orthorhombic TbMnO3 is studied from first principles. We compare the cases in which the spin cycloid, which induces the electric polarization via the spin-orbit interaction, is in either the b-c or a-b plane. We find that the electronic contribution is negligible in the first case, but much larger, and comparable to the lattice-mediated contribution, in the second case. However, we how that this behavior is an artifact of the particular pattern of octahedral rotations characterizing the structurally relaxed Pbnm crystal structure. To do so, we explore how the electronic contribution varies for a structural model of rigidly rotated MnO6 octahedra, and demonstrate that it can vary over a wide range, comparable with the lattice-mediated contribution, for both b-c and a-b spirals. We introduce a phenomenological model that is capable of describing this behavior in terms of sums of symmetry-constrained contributions arising from the displacements of oxygen atoms from the centers of the Mn-Mn bonds.Comment: 8 pages, 5 figures, 3 table

Natural optical activity and its control by electric field in electrotoroidic systems

We propose the existence, via analytical derivations, novel phenomenologies, and first-principles-based simulations, of a new class of materials that are not only spontaneously optically active, but also for which the sense of rotation can be switched by an electric field applied to them-- via an induced transition between the dextrorotatory and laevorotatory forms. Such systems possess electric vortices that are coupled to a spontaneous electrical polarization. Furthermore, our atomistic simulations provide a deep microscopic insight into, and understanding of, this class of naturally optically active materials.Comment: 3 figure