Validity and limitations of the superexchange model for the magnetic properties of Sr2IrO4 and Ba2IrO4 mediated by the strong spin-orbit coupling

Layered perovskites Sr2IrO4 and Ba2IrO4 are regarded as the key materials for understanding the properties of magnetic relativistic insulators, mediated by the strong spin-orbit (SO) coupling. One of the most fundamental issues is to which extent these properties can be described by the superexchange (SE) model, formulated in the limit of the large Coulomb repulsion. In the present work we address this issue by deriving the relevant models and extracting parameters of these models from the first-principles calculations. First, we construct the effective Hubbard-type model for the t2g bands, by recasting the problem in the language of Wannier orbitals. Then, we map the obtained electron model onto the pseudospin model by applying the theory of SE interactions. We discuss the microscopic origin of anisotropic SE interactions, inherent to the compass Heisenberg model, and the appearance of the antisymmetric Dzyaloshinskii-Moriya term, associated with the additional rotation of the IrO6 octahedra in Sr2IrO4. In order to evaluate the Neel temperature (TN), we employ the non-linear sigma model. While for Sr2IrO4 our value of TN agrees with the experimental one, for Ba2IrO4 it is overestimated by a factor two. We argue that this discrepancy is related to limitations of the SE model: while for more localized t2g states in Sr2IrO4 it works reasonably well, the higher-order terms, beyond the SE model, play a more important role in the more "itinerant" Ba2IrO4, giving rise to the new type of isotropic and anisotropic exchange interactions. This conclusion is supported by unrestricted Hartree-Fock calculations for the same electron model, where in the case of Ba2IrO4, already on the mean-field level, we were able to reproduce the experimentally observed magnetic ground state, while for Sr2IrO4 the main results are essentially the same as in the SE model.Comment: 37 pages, 9 figure

Microscopic analysis of the magnetic form factor in low-dimensional cuprates

We analyze the magnetic form factor of Cu$^{2+}$ in low-dimensional quantum magnets by taking the metal-ligand hybridization into account explicitly. In this analysis we use the form of magnetic Wannier orbitals, derived from the first-principles calculations, and identify the contributions of different atomic sites. Having performed local density approximation calculations for cuprates with different types of ligand atoms, we discuss the influence of the on-site Coulomb correlations on the structure of the magnetic orbital. The typical composition of Wannier functions for copper oxides, chlorides and bromides is defined and related to features of the magnetic form factor. We propose easy-to-use approximations of the partial orbital contributions to the magnetic form factor in order to give a microscopic explanation for the results obtained in previous first-principles studies.Comment: 5 pages, 4 figure

Monte Carlo study of magnetic nanoparticles adsorbed on halloysite Al2Si2O5(OH)4Al_2Si_2O_5(OH)_4 nanotubes

We study properties of magnetic nanoparticles adsorbed on the halloysite surface. For that a distinct magnetic Hamiltonian with random distribution of spins on a cylindrical surface was solved by using a nonequilibrium Monte Carlo method. The parameters for our simulations: anisotropy constant, nanoparticle size distribution, saturated magnetization and geometrical parameters of the halloysite template were taken from recent experiments. We calculate the hysteresis loops and temperature dependence of the zero field cooling (ZFC) susceptibility, which maximum determines the blocking temperature. It is shown that the dipole-dipole interaction between nanoparticles moderately increases the blocking temperature and weakly increases the coercive force. The obtained hysteresis loops (e.g., the value of the coercive force) for Ni nanoparticles are in reasonable agreement with the experimental data. We also discuss the sensitivity of the hysteresis loops and ZFC susceptibilities to the change of anisotropy and dipole-dipole interaction, as well as the 3d-shell occupation of the metallic nanoparticles; in particular we predict larger coercive force for Fe, than for Ni nanoparticles.Comment: 10 pages, 12 figure

Profile approach for recognition of three-dimensional magnetic structures

We propose an approach for low-dimensional visualisation and classification of complex topological magnetic structures formed in magnetic materials. Within the approach one converts a three-dimensional magnetic configuration to a vector containing the only components of the spins that are parallel to the z axis. The next crucial step is to sort the vector elements in ascending or descending order. Having visualized profiles of the sorted spin vectors one can distinguish configurations belonging to different phases even with the same total magnetization. For instance, spin spiral and paramagnetic states with zero total magnetic moment can be easily identified. Being combined with a simplest neural network our profile approach provides a very accurate phase classification for three-dimensional magnets characterized by complex multispiral states even in the critical areas close to phases transitions. By the example of the skyrmionic configurations we show that profile approach can be used to separate the states belonging to the same phase

Bimeron nanoconfined design

We report on the stabilization of the topological bimeron excitations in confined geometries. The Monte Carlo simulations for a ferromagnet with a strong Dzyaloshinskii-Moriya interaction revealed the formation of a mixed skyrmion-bimeron phase. The vacancy grid created in the spin lattice drastically changes the picture of the topological excitations and allows one to choose between the formation of a pure bimeron and skyrmion lattice. We found that the rhombic plaquette provides a natural environment for stabilization of the bimeron excitations. Such a rhombic geometry can protect the topological state even in the absence of the magnetic field.Comment: 5 pages, 7 figure

First-principles study of the magnetic ground state in kagome francisites Cu3Bi(SeO3)2O2X (X=Cl, Br)

We explore magnetic behavior of kagome francisites Cu3Bi(SeO3)2O2X (X = Cl and Br) using first-principles calculations. To this end, we propose an approach based on the Hubbard model in the Wannier functions basis constructed on the level of local-density approximation (LDA). The ground-state spin configuration is determined by a Hartree-Fock solution of the Hubbard model both in zero magnetic field and in applied magnetic fields. Additionally, parameters of an effective spin Hamiltonian are obtained by taking into account the hybridization effects and spin-orbit coupling. We show that only the former approach, the Hartree-Fock solution of the Hubbard model, allows for a complete description of the anisotropic magnetization process. While our calculations confirm that the canted zero-field ground state arises from a competition between ferromagnetic nearest-neighbor and antiferromagnetic next-nearest-neighbor couplings in the kagome planes, weaker anisotropic terms are crucial for fixing spin directions and for the overall magnetization process. We thus show that the Hartree-Fock solution of an electronic Hamiltonian is a viable alternative to the analysis of effective spin Hamiltonians when a magnetic ground state and effects of external field are considered

Magnetic frustration in BaCuSi2O6 released

Han Purple (BaCuSi2O6) is not only an ancient pigment, but also a valuable model material for studying Bose-Einstein condensation (BEC) of magnons in high magnetic fields. Using precise low-temperature structural data and extensive density-functional calculations, we elucidate magnetic couplings in this compound. The resulting magnetic model comprises two types of nonequivalent spin dimers, in excellent agreement with the (63,65)Cu nuclear magnetic resonance data. We further argue that leading interdimer couplings connect the upper site of one dimer to the bottom site of the contiguous dimer, and not the upper-to-upper and bottom-to-bottom sites, as assumed previously. This finding is verified by inelastic neutron scattering data and implies the lack of magnetic frustration in BaCuSi2O6, thus challenging existing theories of the magnon BEC in this compound.Comment: 4.5 pages, 4 figures, 1 tabl