First-principles study of pressure effects on and

We have performed first-principles calculations to investigate the pressure effects on CaFe₂As₂ and BaFe₂As₂. Our calculations show that in CaFe₂As₂, the orthorhombic structure transforms to a collapsed tetragonal structure at 0.4 GPa with a volume collapse of 9.5%, which is in agreement with experiments. Together with the structural phase transition, CaFe₂As₂ undergoes a magnetic transition from the stripe antiferromagnetic ordering to the nonmagnetic state. For BaFe₂As₂, we predict that the orthorhombic structure transforms to the tetragonal structure at 9.4 GPa. Unlike CaFe₂As₂, the magnetic moments of Fe ions in BaFe₂As₂ are not zero and the stripe antiferromagnetic ordering transforms to the checkerboard antiferromagnetic ordering together with the structural phase transition. The stability of the orthorhombic structure up to 9.4 GPa suggests that superconductivity and magnetism coexist in BaFe₂As₂.     

Correction: Ab initio study of anisotropic mechanical and electronic properties of strained carbon-nitride nanosheet with interlayer bonding

The magnetic and electronic properties of strontium titanate with different carbon dopant configurations are explored using first-principles calculations with a generalized gradient approximation (GGA) and the GGA+U approach. Our results show that the structural stability, electronic properties and magnetic properties of C-doped SrTiCO₃ strongly depend on the distance between carbon dopants. In both GGA and GGA+U calculations, the doping structure is mostly stable with a nonmagnetic feature when the carbon dopants are nearest neighbors, which can be ascribed to the formation of a C-C dimer pair accompanied by stronger C-C and weaker C-Ti hybridizations as the C-C distance becomes smaller. As the C-C distance increases, C-doped SrTiCO₃ changes from an n-type nonmagnetic metal to ferromagnetic/antiferromagnetic half-metal and to an antiferromagnetic/ferromagnetic semiconductor in GGA calculations, while it changes from a nonmagnetic semiconductor to ferromagnetic half-metal and to an antiferromagnetic semiconductor using the GGA+U method. Our work demonstrates the possibility of tailoring the magnetic and electronic properties of C-doped SrTiO₃, which might provide some guidance to extend the applications of strontium titanate as a magnetic or optoelectronic material.

     

Vacancy induced magnetism in SrTiO3

Vacancy-induced magnetism in perovskite SrTiO₃ is investigated by ab initio calculations and magnetic measurements. The calculations of the generalized gradient approximation (GGA), the local density approximation (LDA) and the local density approximation with on-site effect U (LDA+U) methods show that stoichiometric SrTiO₃ is nonmagnetic. The GGA calculated results indicate that Ti or O vacancy could induce magnetism rather than Sr vacancy. The LDA and LDA+U calculations show that the Ti vacancy could induce magnetism, while Sr and O vacancies couldn't. The experimental results confirm that SrTiO₃ nanocrystalline powders exhibit room-temperature ferromagnetism (FM) and the magnetic moment results from cation vacancies.     

KCrF3中的轨道有序及其成因

强关联体系中的轨道有序及其成因一直是凝聚态物理研究的热点问题.轨道有序对于巨磁阻和 超导材料的研究有非常重要的地位.利用第一性原理计算研究了KCrF₃的四方相和立方相中的轨道有序 及其成因.在四方相中, GGA和GGA+U两种方法计算结果都表明其基态是A型反铁磁和G型轨道有序. 对于立方结构, GGA方法得出铁磁半金属态是基态,而GGA+U(U_eff = 3.0 eV)得到的基态是A型 反铁磁绝缘体. 光电导测量是少数能从实验上观察到轨道有序的方法之一,因此计算了其光电导,并结合投影态密度讨论 了KCrF₃中的轨道有序.最后找到了其轨道有序的成因:电子强关联效应,而非电-声子相互作用是其 轨道 有序的物理根源.     

Magnetism of Fe in SrFe2As2: Local investigation by time differential perturbed angular distribution (TDPAD) spectroscopy

Employing the γ-ray perturbed angular distribution technique, we have measured the magnetic hyperfine field of ⁵⁴Fe in tetragonal and orthorhombic structural phases of SrFe₂As₂. In the tetragonal phase, the magnetic response of ⁵⁴Fe shows Curie-Weiss type local susceptibility, indicating the presence of localized moment on Fe. The temperature dependence of the hyperfine field of ⁵⁴Fe reflects quasi-two dimensional first order magnetic transition at 200 K. Our data indicate that Fe moments in the magnetically ordered phase of SrFe₂As₂ may be canted out of the ab-plane.     

Ferromagnetic origin of Na and Mn codoped CaZn<Subscript>2</Subscript>As<Subscript>2</Subscript> diluted magnetic semiconductor: A first-principles study

We have investigated the electronic structure and magnetic properties of Na and Mn codoped CaZn₂As₂ using density functional theory within the generalized gradient approximation (GGA)+U schemes. We have shown that the ground state magnetic structure of Mn-doped CaZn₂As₂ is antiferromagnetic while holemediated Zener’s p–d exchange is responsible for the origin of ferromagnetism of Na and Mn codoped CaZn₂As₂.     

First-principles studies on the structural and electronic properties of Li-ion battery cathode material CuF2

The 3d transition metal binary compounds have been extensively investigated for a large multi-electron redox capacity through reversible electrochemical reactions. Here, the structural, electronic and magnetic properties of CuF₂ are studied by the first-principles calculations within both the generalized gradient approximation (GGA) and GGA+U frameworks. Our results show that the antiferromagnetic (AFM) configuration of CuF₂ is more stable than the ferromagnetic (FM) one, which is consistent with experiments. The analysis of the electronic density of states (DOS) shows that CuF₂ is a classic Mott–Hubbard insulator with a large d–d type band gap, which is similar to the case of FeF₃. Moreover, small spin polarizations were found on the sites of fluorin ions, which accords with a fluorin-mediated superexchange mechanism for the Cu–Cu magnetic interaction.     

First-principles linear muffin-tin orbital investigations in the electronic and magnetic structures of double perovskites Ba2TMoO6 (T=V,Cr, Mn,Fe and Co)

The electronic and magnetic structures of ordered double perovskites Ba₂TMoO₆ (T=V, Cr, Mn, Fe and Co) are systematically investigated by means of the first-principle linear muffin-tin orbitals with the atomic-sphere approximation (LMTO-ASA) method. The calculations are performed by using the both local spin density approximation (LSDA) and the LSDA+U Coulomb interaction schemes. The results show a half-metallic ferrimagnetic ground states for T=Cr, Fe and Co in LSDA+U treatment, whereas half-metallic ferromagnetic character is observed for T=V. For T=Mn, insulating ground state is obtained, stabilized in the antiferromagnetic state. The LSDA+U calculations yield better agreement with the theoretical and the experimental results than do the LSDA.     

Antiferromagnetic and semiconducting material CrNCN: Prediction from first-principles investigation

The structural stability and physical properties of CrNCN were studied using density functional theory with explicit electronic correlation (GGA+U). Calculated results indicate that the title compound, similar to MNCN (M=Mn, Fe, Co, Ni), is thermodynamically stable but mechanically unstable. Analysis of electronic and magnetic structures reveals that CrNCN is an antiferromagnetic semiconductor. However, the exact magnetic structure of CrNCN consists of an antiferromagnetic intralayer and a ferromagnetic interlayer, which differs from that of the type-II antiferromagnetic semiconductor MNCN (M=Mn, Fe, Co, Ni), which consists of a ferromagnetic intralayer and an antiferromagnetic interlayer.     

Ab initio study of the structural,electronic, elastic and magnetic properties of Cu2GdIn,Ag2GdIn and Au2GdIn

We preformed first-principle calculations for the structural, electronic, elastic and magnetic properties of Cu₂GdIn, Ag₂GdIn and Au₂GdIn using the full-potential linearized augmented plane wave (FP-LAPW) scheme within the generalized gradient approximation by Wu and Cohen (GGA-WC), GGA+U, the local spin density approximation (LSDA) and LSDA+U. The lattice parameters, the bulk modulus and its pressure derivative and the elastic constants were determined. Also, we present the band structures and the densities of states. The electronic structures of the ferromagnetic configuration for Heusler compounds (X₂GdIn) have a metallic character. The magnetic moments were mostly contributed by the rare-earth Gd 4f ion.     

Charge and spin dynamics in antiferromagnetic metallic phase of iron-based superconductors

The electronic states, charge dynamics, and spin dynamics in the antiferromagnetic metallic phase of iron-arsenide superconductors are investigated by mean-field calculations for a five-band Hubbard model. Taking into account the difference of observed magnetic moments between LaFeAsO (1111 system) and BaFe₂As₂ (122 system), we investigate the effect of the magnitude of the moments on band dispersion, optical conductivity, and dynamical spin susceptibility. We clarify how the magnitude affects on these quantities and predict different behaviors between the 1111 and 122 systems in the antiferromagnetic metallic phase.     

New superconducting RbFe2As2: A first-principles investigation

RbFe₂As₂ has recently been reported to be a bulk superconductor with T_c = 2.6 K in the undoped state, in contrast to undoped BaFe₂As₂ with a magnetic ground state. We present here the results of the first-principles calculations of the structural, elastic and electronic properties for this newest superconductor and discuss its behaviour in relation to other related systems.     

First-principles study of ferromagnetism in Zn- and Cd-doped SnO2

The electronic structures and magnetic properties of Zn- and Cd-doped SnO₂ are investigated using first-principles calculations within the generalized gradient approximation (GGA) and GGA+U scheme. The substitutional Zn and Cd atoms introduce holes in the 2p orbitals of the O atoms and the introduced holes are mostly confined to the minority-spin states. The magnetic moment induced by doping mainly comes from the 2p orbitals of the O atoms, among which the moment of the first neighboring O atoms around the dopant are the biggest. The U correction for the anion-2p states obviously increases the moment of the first neighboring O atoms and transforms the ground states of the doped SnO₂ from half-metallic to insulating. The magnetic coupling between the moments induced by two dopants is ferromagnetic and the origin of ferromagnetic coupling can be attributed to the p–d hybridization interaction involving holes.     

Fe K-edge X-ray resonant magnetic scattering from Ba(Fe1?xCox)2As2 superconductors

We present an X-ray resonant magnetic scattering study at the Fe-K absorption edge of the BaFe₂As₂ compound. The energy spectrum of the resonant scattering, together with our calculation using the full-potential linear-augmented plane wave method with a local density functional suggests that the observed resonant scattering arises from electric dipole (E1) transitions. We discuss the role of Fe K-edge X-ray resonant magnetic scattering in understanding the relationship between the structure and the antiferromagnetic transition in the doped Ba(Fe_1−x Co _x )₂As₂ superconductors.     

W形六角铁氧体BaFe18O27电子结构与导电性的第一性原理研究

采用基于第一性原理的GGA+U方法研究了BaFe₁₈O₂₇的晶体结构和基态电子结构. 以实验数据为初始结构的离子弛豫显示,由于稳定结构中离子半径的差异和2d位Fe的存在,位于BaO层中6h位的O离子脱离了实验结构中原胞的"表面"位置,产生畸变. 计算得到晶体磁矩为28 μ_B/f.u.,与实验相符. 电子态密度及能带计算表明该材料具有微弱的半金属特性,而且与c轴平行方向和垂直方向的能带色散关系有着很大不同,6g位Fe在该材料的输运特性中起着关键作用,它们形成一种"导电层",导致垂直电导率和平行电导率出现非常大的差异. 关键词： 第一性原理 W形六角铁氧体 电子结构 导电性     

Potential parent compound of superconductor: Sr2CuM2As2O2 (M = Mn, Fe)

The electronic structure of Sr₂CuMn₂As₂O₂ and Sr₂CuFe₂As₂O₂ are studied by the first-principle calculations. These compounds have a body-centered-tetragonal crystal structure that consists of the CuO₂ layers similar to those in the high-Tc cuprate superconductor, and intermetallic MAs (M = Mn, or Fe) layers similar to the FeAs layers in high-Tc pnictides. Such special structure makes them as interesting candidates for new type of superconductor since they have two types of superconducting layers. However, our calculations indicate that the states in the range from −2.0 eV to +2.0 eV are dominated by Mn-3d or Fe-3d states, while the states of Cu-3d are far away from the Fermi level (in the range from −3.0 eV to −1.0 eV). Such results are significantly different with the Cu-based superconductor, like La₂CuO₄, where the states around Fermi level are dominated by Cu-3d states. Besides, we find that the mean-field magnetic ground state is the checkerboard antiferromagnetic in Cu sublattice and the stripe antiferromagnetic in Fe (or Mn) sublattice.     

The role of Co impurities and oxygen vacancies in the ferromagnetism of Co-doped SnO2: GGA and GGA+U studies

The electronic structure and ferromagnetic stability of Co-doped SnO₂ are studied using the first-principle density functional method within the generalized gradient approximation (GGA) and GGA+U schemes. The addition of effective U_Co transforms the ground state of Co-doped SnO₂ to insulating from half-metallic and the coupling between the nearest neighbor Co spins to weak antimagnetic from strong ferromagnetic. GGA+U_Co calculations show that the pure substitutional Co defects in SnO₂ cannot induce the ferromagnetism. Oxygen vacancies tend to locate near Co atoms. Their presence increases the magnetic moment of Co and induces the ferromagnetic coupling between two Co spins with large Co-Co distance. The calculated density of state and spin density distribution calculated by GGA+U_Co show that the long-range ferromagnetic coupling between two Co spins is mediated by spin-split impurity band induced by oxygen vacancies. More charge transfer from impurity to Co-3d states and larger spin split of Co-3d and impurity states induced by the addition of U_Co enhance the ferromagnetic stability of the system with oxygen vacancies. By applying a Coulomb U_O on O 2 s orbital, the band gap is corrected for all calculations and the conclusions derived from GGA+U_Co calculations are not changed by the correction of band gap.     

Electronic structure of new iron-based superconductors: From pnictides to chalcogenides and other similar systems

The electronic spectra of new iron-based high-temperature superconductors and a number of other chemically similar compounds have been discussed and compared with the focus on iron chalcogenide K_{1 ? x} Fe_{2 ? y} Se₂ and isostructural pnictide BaFe₂As₂ (122). It has been shown that the Fermi surfaces in K_{1 ? x} Fe_{2 ? y} Se₂ are significantly different from those in pnictides. The LDA + DMFT and LDA’ + DMFT calculations have demonstrated that the effect of electron correlations in K_{1 ? x} Fe_{2 ? y} Se₂ on the electronic structure is much stronger than that in the most studied 122 system. The electronic structure of several multiband superconductors similar in chemical composition to iron-based high-temperature superconductors, but having a relatively low T _c value (such as SrPt₂As₂, APt₃P (A = Sr, Ca, La), and (Sr, Ca)Pd₂As₂), and the non-superconducting compound BaFe₂Se₃ has also been discussed. It has been shown that the electronic structure of these systems is significantly different from previously studied iron pnictides and chalcogenides. The T _c value in these systems can be understood within the simple Bardeen-Cooper-Schrieffer model.     

Electronic structure of Zn in oxide spinels

Using⁶⁷Zn Mössbauer absorption and emission spectroscopy, we have investigated the electronic structure at the A and B sites in the normal spinels (Zn)[Al₂]O₄, (Zn)[Fe₂]O₄ and (Zn)[Ga₂]O₄. Within each system, the center shift S_c at the A site is more positive. In all systems investigated, the electric field gradientV _u at the B site is negative. The values for S_C andV _U scale with oxygen nearest-neighbour distance to Zn. In the Fe spinel, a transferred magnetic hyperfine field is observed at the Zn site below the antiferromagnetic ordering temperatureT _N=10 K. For a more detailed discussion of the chemical bond, we have performed ab initio Hartree-Fock cluster calculations for the Al and Fe spinels. Our experimental and theoretical results show that all hyperfine parameters are essentially determined by covalency effects. Our data on the Ga spinel raise the question of a partially inverse structure.     

Electronic and magnetic properties of Fe<Subscript>2</Subscript>SiC

The electronic structure and magnetic properties of Fe₂SiC compound have been studiedusing the framework of an all-electron full-potential linearized augmented-plane wave(FP-LAPW) method within the local density (LSDA) and + U corrected(LSDA + U)approximations. An antiferromagnetic spin ordering of Fe atoms is shown to be the groundstate for this compound. From the electronic band structures and density of states (DOS),Fe₂SiC has ametallic character and from the analysis of the site and momentum projected densities, itis deduced that the bonding is achieved through hybridization of Fe-3d with C-2p states andFe-3d withSi-3pstates. It is also pointed out that the Fe-C bonding is more covalent than Fe-Si. In theFM phase, the spin polarized calculations indicate that the total magnetic moment ofFe₂SiC increasesfrom 0.41 to 4.33μ _B when the Hubbard U parameter for iron isconsidered.