Ab initio Derivation of Low-Energy Model for Alkali-Cluster-Loaded Sodalites

An effective low-energy model describing magnetic properties of alkali-cluster-loaded sodalites is derived by {\em ab initio} downfolding. We start with constructing an extended Hubbard model for maximally localized Wannier functions. {\em Ab initio} screened Coulomb and exchange interactions are calculated by constrained random phase approximation. We find that the system resides in the strong coupling regime and thus the Heisenberg model is derived as a low-energy model of the extended Hubbard model. We obtain antiferromagnetic couplings $\sim$ $O$(10 K), being consistent with the experimental temperature dependence of the spin susceptibility. Importance of considering the screening effect in the derivation of the extended Hubbard model is discussed.Comment: 9 pages, 5 figures, 2 table

Control of Dzyaloshinskii-Moriya interaction in Mn1−x_{1-x}Fex_xGe: a first-principles study

Motivated by the recent experiment on the size and helicity control of skyrmions in Mn$_{1-x}$Fe$_x$Ge [K. Shibata et al., Nature Nanotechnology 8, 732 (2013)], we study how the Dzyaloshinskii-Moriya (DM) interaction changes its size and sign in metallic helimagnets. By means of first-principles calculations, we successfully reproduce the non-trivial sign change of the DM interaction observed in the experiment. While the DM interaction sensitively depends on the carrier density or the detail of the electronic structure such as the size of the exchange splitting, its behavior can be systematically understood in terms of the distribution of anticrossing points in the band structure. By following this guiding principle, we can even induce gigantic anisotropy in the DM interaction by applying a strain to the system. These results pave the new way for skyrmion crystal engineering in metallic helimagnets.Comment: 7 pages, 8 figures, 1 tabl

First-Principles Evaluation of the Dzyaloshinskii--Moriya Interaction

We review recent developments of formulations to calculate the Dzyaloshinskii--Moriya (DM) interaction from first principles. In particular, we focus on three approaches. The first one evaluates the energy change due to the spin twisting by directly calculating the helical spin structure. The second one employs the spin gauge field technique to perform the derivative expansion with respect to the magnetic moment. This gives a clear picture that the DM interaction can be represented as the spin current in the equilibrium within the first order of the spin-orbit couplings. The third one is the perturbation expansion with respect to the exchange couplings and can be understood as the extension of the Ruderman--Kittel--Kasuya--Yosida (RKKY) interaction to the noncentrosymmetric spin-orbit systems. By calculating the DM interaction for the typical chiral ferromagnets Mn$_{1-x}$Fe$_x$Ge and Fe$_{1-x}$Co$_x$Ge, we discuss how these approaches work in actual systems.Comment: invited review pape

Electronic Structure Calculation and Superconductivity in λ\lambda-(BETS)2_{2}GaCl4_{4}

Quasi-two-dimensional molecular conductor $\lambda$-(BETS)$_2$GaCl$_4$ shows superconductivity (SC) below 5.5K, neighboring the dimer-type Mott insulating phase. To elucidate the origin of SC and its gap function, we carry out first-principles band calculation and derive a four-band tight-binding model from the maximally localized Wannier orbitals. Considering the spin-fluctuation-mediated mechanism by adding the Hubbard $U$-term to the model, we analyze the SC gap function by applying the random phase approximation. We show that the SC gap changes its sign four times along the Fermi surface (FS) in the unfolded Brillouin zone, suggestive of a $d$-wave-like SC gap, which only has two-fold symmetry because of the low symmetry of the crystal structure. Decomposing the SC gap into the pairing functions along the crystal axes, we compare the result to similar analysis of the well-studied $\kappa$-type molecular conductors and to the experiments.Comment: 5 pages, 2 figures, 3 table

Doppler shift picture of the Dzyaloshinskii--Moriya interaction

We present a physical picture for the emergence of the Dzyaloshinskii--Moriya (DM) interaction based on the idea of the Doppler shift by an intrinsic spin current induced by spin--orbit interaction under broken inversion symmetry. The picture is confirmed by a rigorous effective Hamiltonian theory, which reveals that the DM coefficient is given by the magnitude of the intrinsic spin current. The expression is directly applicable to first principles calculations and clarifies the relation between the interaction and the electronic band structures. Quantitative agreement with experimental results is obtained for the skyrmion compounds Mn$_{1-x}$Fe$_x$Ge and Fe$_{1-x}$Co$_x$Ge.Comment: 5 pages, 4 figures; v2 references adde

In-plane electric polarization of bilayer graphene nanoribbons by interlayer bias voltage

We theoretically show that an interlayer bias voltage in the AB-stacked bilayer graphene nanoribbons with armchair edges induces an electric polarization along the ribbon. Both tight-binding and ab initio calculations consistently indicate that when the bias voltage is weak, the polarization shows opposite signs depending on the ribbon width modulo three. This nontrivial dependence is explained using a two-band effective model. A strong limit of the bias voltage in the tight-binding model shows either one-third or zero polarization, which agrees with topological argument.Comment: 11 pages, 9 figures, accepted by PR

Effect of van Hove singularities on high-Tc superconductivity in H3S

One of interesting open questions for the high transition temperature (Tc) superconductivity in sulfur hydrides is why high pressure phases of H3S have extremely high Tc's. Recently, it has been pointed out that the presence of the van Hove singularities (vHs) around the Fermi level is crucial. However, while there have been quantitative estimates of Tc based on the Migdal-Eliashberg theory, the energy dependence of the density of states (DOS) has been neglected to simplify the Eliashberg equation. In this study, we go beyond the constant DOS approximation and explicitly consider the electronic structure over 40eV around the Fermi level. In contrast with the previous conventional calculations, this approach with a sufficiently large number of Matsubara frequencies enables us to calculate Tc without introducing the empirical pseudo Coulomb potential. We show that while H3S has much higher Tc than H2S for which the vHs is absent, the constant DOS approximation employed so far seriously overestimates (underestimates) Tc by ~ 60K (~ 10K) for H3S (H2S). We then discuss the impact of the strong electron-phonon coupling on the electronic structure with and without the vHs and how it affects the superconductivity. Especially, we focus on (1) the feedback effect in the self-consistent calculation of the self-energy, (2) the effect of the energy shift due to the zero-point motion, and (3) the effect of the changes in the phonon frequencies due to strong anharmonicity. We show that the effect of (1)-(3) on Tc is about 10-30K for both H3S and H2S. Eventually, Tc is estimated to be 181K for H3S at 250GPa and 34K for H2S at 140GPa, which explains the pressure dependence of Tc observed in the experiment. In addition, we evaluate the lowest order vertex correction beyond the Migdal-Eliashberg theory and discuss the validity of the Migdal approximation for sulfur hydrides

Formation mechanism of helical Q structure in Gd-based skyrmion materials

Using the ab initio local force method, we investigate the formation mechanism of the helical spin structure in GdRu$_2$Si$_2$ and Gd$_2$PdSi$_3$. We calculate the paramagnetic spin susceptibility and find that the Fermi surface nesting is not the origin of the incommensurate modulation, in contrast to the naive scenario based on the Ruderman-Kittel-Kasuya-Yosida mechanism. We then decompose the exchange interactions between the Gd spins into each orbital component, and show that spin-density-wave type interaction between the Gd-5$d$ orbitals is ferromagnetic, but the interaction between the Gd-4$f$ orbitals is antiferromagnetic. We conclude that the competition of these two interactions, namely, the inter-orbital frustration, stabilizes the finite-Q structure.Comment: 5 pages, 4 figure

Local force method for the ab initio tight-binding model with spin-dependent hopping

To estimate the Curie temperature of metallic magnets from first principles, we develop a local force method for the tight-binding model having spin-dependent hopping derived from spin density functional theory. While spin-dependent hopping is crucial for the self-consistent mapping to the effective spin model, the numerical cost to treat such non-local terms in the conventional Green's function scheme is formidably expensive. Here, we propose a formalism based on the kernel polynomial method (KPM), which makes the calculation dramatically efficient. We perform a benchmark calculation for bcc-Fe, fcc-Co, and fcc-Ni and find that the effect of the magnetic non-local terms is particularly prominent for bcc-Fe. We also present several local approximations to the magnetic non-local terms for which we can apply the Green's function method and reduce the numerical cost further by exploiting the intermediate representation of the Green's function. By comparing the results of the KPM and local methods, we discuss which local method works most successfully. Our approach provides an efficient way to estimate the Curie temperature of metallic magnets with a complex spin configuration.Comment: 10 pages, 3 figure

Field-direction control of the type of charge carriers in nonsymmorphic IrO2

In the quest for switching of the charge carrier type in conductive materials, we focus on nonsymmorphic crystals, which are expected to have highly anisotropic folded Fermi surfaces due to the symmetry requirements. Following simple tight-binding model simulation, we prepare nonsymmorphic IrO2 single-crystalline films with various growth orientations by molecular beam epitaxy, and systematically quantify their Hall effect for the corresponding field directions. The results clearly demonstrate that the dominant carrier type can be intrinsically controlled by the magnetic field direction, as also evidenced by first-principles calculations revealing nontrivial momentum dependence of the group velocity and mass tensor on the folded Fermi surfaces and its anisotropic nature for the field direction.Comment: 12 pages, 4 figure