Electronic structure of prototype AFe<Subscript>2</Subscript>As<Subscript>2</Subscript> and ReOFeAs high-temperature superconductors: A comparison

We have performed ab initio LDA calculations of the electronic structure of newly discovered prototype high-temperature superconductors AFe₂As₂ (A = Ba, Sr) and compared it with the previously calculated electronic spectra of ReOFeAs (Re = La, Ce, Pr, Nd, Sm). In all cases, we obtain almost identical densities of states in a rather wide energy interval (up to 1 eV) around the Fermi level. Energy dispersions are also very similar and almost two dimensional in this energy interval, leading to the same basic (minimal) model of the electronic spectra, determined mainly by Fe d orbitals of the FeAs layers. The other constituents, such as A ions or rare-earth Re (or oxygen states) are more or less irrelevant for superconductivity. LDA Fermi surfaces for AFe₂As₂ are also very similar to that of ReOFeAs. This makes the more simple AFe₂As₂ a generic system to study the high-temperature superconductivity in FeAs-layered compounds. The text was submitted by the authors in English.     

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.     

Hyperfine interactions and electronic structures of BaFe 2 As 2 : a first-principles LDA+U study

The hyperfine parameters of hyperfine fields, electric field gradients and isomer shifts at the Fe site are investigated based on the first-principles calculations of the electronic structures using LDA (GGA)+U method in the low-temperature orthorhombic antiferromagnetic phase of undoped BaFe₂As₂. It is fond that the electric field gradient of Fe nucleus is highly related with the electronic structures close to the Fermi level. Though the addition of negative on-site Coulomb interaction to Fe-3d states improves the calculated magnetic moment of Fe atom and the hyperfine parameters of Fe nucleus when U = ?0.1 Ry (?0.08 Ry) for GGA+U (LDA+U) method, a negative U correction does not capture the right physics of this system. The calculations prove the strong coupling between the magnetic, structural and electronic properties in antiferromagnetic BaFe₂As₂ parent.     

Electronic structure of new multiple band Pt-pnictide superconductors APt3P

We report LDA calculated band structure, densities of states and Fermi surfaces for recently discovered Pt-pnictide superconductors APt₃P (A = Ca, Sr, La), confirming their multiple band nature. Electronic structure is essentially three dimensional, in contrast to Fe pnictides and chalcogenides. LDA calculated Sommerfeld coefficient agrees rather well with experimental data, leaving little space for very strong coupling super-conductivity, suggested by experimental data on specific heat of SrPt₃P. Elementary estimates show, that the values of critical temperature can be explained by rather weak or moderately strong coupling, while the decrease in superconducting transition temperature T _c from Sr to La compound can be explained by corresponding decrease in total density of states at the Fermi level N(E _F). The shape of the density of states near the Fermi level suggests that in SrPt₃P electron doping (such as replacement Sr by La) decreases N(E _F) and T _c , while hole doping (e.g., partial replacement of Sr with K, Rb or Cs, if possible) would increase N(E _F) and possibly T _c .     

Electronic structure of novel multiple-band superconductor SrPt<Subscript>2</Subscript>As<Subscript>2</Subscript>

The electronic structure of the recently discovered superconductor SrPt₂As₂ with T _c = 5.2 K has been calculated in the local-density approximation. Despite its chemical composition and crystal structure are somehow similar to FeAs-based high-temperature superconductors, the electronic structure of SrPt₂As₂ is very much different. The crystal structure is orthorhombic (or tetragonal if idealized) and has layered nature with alternating PtAs₄ and AsPt₄ tetrahedra slabs sandwiched with Sr ions. The Fermi level is crossed by Pt-5d states with rather strong admixture of As-4p states. Fermi surface of SrPt₂As₂ is essentially three-dimensional, with complicated sheets corresponding to multiple bands. We compare SrPt₂As₂ with 1111 and 122 representatives of FeAs-class of superconductors, as well as with isovalent (Ba,Sr)Ni₂As₂ superconductors. Brief discussion of superconductivity in SrPt₂As₂ is also presented.     

Charge transfer effects on the Fermi surface of Ba0.5K0.5Fe2As2

Ab‐initio calculations within density functional theory are performed to obtain a more systematic understanding of the electronic structure of iron pnictides. As a prototypical compound we study Ba_0.5K_0.5Fe₂As₂ and analyze the changes of its electronic structure when the interaction between the Fe₂As₂ layers and their surrounding is modified. We find strong effects on the density of states near the Fermi energy as well as the Fermi surface. The role of the electron donor atoms in iron pnictides thus cannot be understood in a rigid band picture. Instead, the bonding within the Fe₂As₂ layers reacts to a modified charge transfer from the donor atoms by adapting the intra‐layer Fe‐As hybridization and charge transfer in order to maintain an As^3‐ valence state.     

Anion height dependence of <Emphasis Type="Italic">T</Emphasis><Subscript><Emphasis Type="Italic">c</Emphasis></Subscript> and the density of states in iron-based superconductors

Systematic ab initio LDA calculations were performed for all the typical representatives of recently discovered class of iron-based high-temperature superconductors: REOFe(As,P) (RE = La, Ce, Nd, Sm, Tb), Ba₂Fe₂As, (Sr,Ca)FFeAs, Sr₄Sc₂O₆Fe₂P₂, LiFeAs and Fe(Se,Te). Non-monotonic behavior of total density of states at the Fermi level is observed as a function of anion height relative to Fe layer with maximum at about Δz _a ～ 1.37 Å, attributed to changing Fe-As (P, Se, Te) hybridization. This leads to a similar dependence of superconducting transition temperature T _c as observed in the experiments. The fit of this dependence to elementary BCS theory produces semiquantitative agreement with experimental data for T _c for the whole class of iron-based superconductors. The similar fit to Allen-Dynes formula underestimates T _c in the vicinity of the maximum, signifying the possible importance of non-phonon pairing in this region. These results unambiguously demonstrate that the main effect of T _c variation between different types of iron-based superconductors is due to the corresponding variation of the density of states at the Fermi level.     

Electronic structure of new AFFeAs prototype of iron arsenide superconductors

This work is provoked by recent discovery of new class prototype systems AFFeAs (A = Sr, Ca) of novel layered ironpnictide High-T _c superconductors (T _c = 36 K). Here we report ab initio LDA results for electronic structure of the AFFeAs systems. We provide detailed comparison between electronic properties of both new systems and reference LaOFeAs (La111) compound. In the vicinity of the Fermi level all three systems have essentially the same band dispersions. However for iron fluoride systems F(2p) states were found to be separated in energy from As(4p) ones in contrast to La111, where O(2p) states strongly overlaps with As(4p). Thus it should be more plausible to include only Fe(3d) and As(4p) orbitals into a realistic noninteracting model than for La111. Moreover Sr substitution with smaller ionic radius Ca in AFFeAs materials leads to a lattice contruction and stronger Fe(3d)-As(4p) hybridization resulting in smaller value of the density of states at the Fermi level in the case of Ca compound. So to some extend Ca system reminds RE111 with later Rare Earths. However Fermi surface of new fluorides is found to be nearly perfect two-dimensional. Also we do not expect strong dependence of superconducting properties with respect to different types of A substitutes. The article is published in the original.     

Electronic structure of new LiFeAs high-T c superconductor

We present results of ab initio LDA calculations of electronic structure of “next generation” layered iron-pnictide high-T _c superconductor LiFeAs (T _c = 18 K). Obtained electronic structure of LiFeAs very similar to recently studied ReOFeAs (Re = La, Ce, Pr, Nd, Sm) and AFe₂As₂ (A = Ba, Sr) compounds. Namely close to the Fermi level its electronic properties are also determined mainly by Fe 3d-orbilats of FeAs₄ two-dimensional layers. Band dispersions of LiFeAs are very similar to the LaOFeAs and BaFe₂As₂ systems as well as the shape of the Fe-3d density of states and Fermi surface. The article is published in the original.     

Electronic structure of Ti-doped Sr<Subscript>4</Subscript>Sc<Subscript>2</Subscript>Fe<Subscript>2</Subscript>As<Subscript>2</Subscript>O<Subscript>6</Subscript> as a possible parent phase for the new FeAs superconductors

First principle FLAPW-GGA calculations have been performed with the purpose to understand the effect of Ti-doping on the electronic properties for the newly discovered tetragonal iron arsenide-oxide Sr₄Sc₂Fe₂As₂O₆ (abbreviated as FeAs42226) as the possible parent phase for the new FeAs superconductors. Our results show that the insertion of Ti into Sc sublattice of this five-component iron arsenide-oxide phase leads to the resolute change of electronic structure of FeAs42226. Namely, the insulating oxygen-containing [Sr₄Sc₂O₆] blocks in Ti-doped FeAs42226 became conducting, and this differs essentially from the known picture for all others FeAs superconductors where the conducting [Fe₂As₂] blocks are alternated with insulating blocks. Moreover in sharp contrast with FeAs-based superconductors with Fe 3d bands near the Fermi level, for Ti-doped FeAs42226 in this region the Ti 3d states are dominated, whereas the Fe 3d states are suppressed.     

Electronic structure reconstruction of CaFe2As2 in the spin density wave state

The electronic structure of CaFe₂As₂, a parent compound of iron-based superconductors, is studied with high-resolution angle-resolved photoemission spectroscopy. The electronic structure of CaFe₂As₂ in the paramagnetic state is consistent with that of density-functional theory calculations. We show that the electronic structure of this compound is significantly reconstructed when entering the spin density wave state. We could resolve two hole-like pockets and four electron-like pockets around the (0, 0) point, and one electron-like pocket surrounded with a pair of electron- and hole-like pockets around the (π, π) point in the spin density wave state. Therefore, the complicated Fermi surface topology and electronic structure near Fermi surface of CaFe₂As₂ illustrate that there exists unconventional electronic reconstruction in the spin density wave state, which cannot be explained by the band folding and Fermi surface nesting pictures.     

Electronic structure,topological phase transitions and superconductivity in (K,Cs)<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript>Fe<Subscript>2</Subscript>Se<Subscript>2</Subscript>

We present LDA band structure of novel hole doped high temperature superconductors (T _c ∼ 30 K) K _x Fe₂Se₂ and Cs _x Fe₂Se₂ and compare it with previously studied electronic structure of isostructural FeAs superconductor BaFe₂As₂ (Ba122). We show that stoichiometric KFe₂Se₂ and CsFe₂Se₂ have rather different Fermi surfaces as compared with Ba122. However at about 60% of hole doping Fermi surfaces of novel materials closely resemble those of Ba122. In between these dopings we observe a number of topological Fermi surface transitions near the Γ point in the Brillouin zone. Superconducting transition temperature T _c of new systems is apparently governed by the value of the total density of states (DOS) at the Fermi level.     

Effect of correlations and doping on the spin susceptibility of iron pnictides: the case of KFe2As2

The temperature dependence of the paramagnetic susceptibility of the iron pnictide superconductor KFe₂As₂ and its connection with the spectral properties of that material is investigated by a combination of density functional theory (DFT) in the local density approximation and dynamical mean-field theory (DMFT). Unlike other iron pnictide parent compounds where the typical oxidation state of iron is 2, the formal valence of Fe in KFe₂As₂ is 2.5, corresponding to an effective doping with 0.5 hole per iron atom compared to, for example, BaFe₂As₂. This shifts the chemical potential and thereby reduces the distance between the peaks in the spectral functions of KFe₂As₂ and the Fermi energy as compared to BaFe₂As₂. The shift, which is clearly seen on the level of DFT as well as in DMFT, is further enhanced by the strong electronic correlations in KFe₂As₂. In BaFe₂As₂ the presence of these peaks results (Phys. Rev. B 86, 125124 (2012)) in a temperature increase in the susceptibility up to a maximum at ～1000 K. While the temperature increase was observed experimentally the decrease at even higher temperatures is outside the range of experimental observability. We show that in KFe₂As₂ the situation is different. Namely, the reduction of the distance between the peaks and the Fermi level due to doping shifts the maximum in the susceptibility to much lower temperatures, such that the decrease in the susceptibility becomes visible in experiment.     

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.     

Electronic and magnetic structure of a possible iron based superconductor BaFe<Subscript>2</Subscript>Se<Subscript>3</Subscript>

We present results of LDA calculations (band structure, densities of states, Fermi surfaces) for possible iron based superconductor BaFe₂Se₃ (Ba123) in normal (paramagnetic) phase. Results are briefly compared with similar data on prototype BaFe₂As₂ and (K,Cs)Fe₂Se₂ superconductors. Without doping this system is anti-ferromagnetic with T _N^exp ∼ 250 K and rather complicated magnetic structure. Neutron diffraction experiments indicated the possibility of two possible spin structures (antiferromagnetically ordered “plaquettes” or “zigzags”), indistinguishable by neutron scattering. Using LSDA calculated exchange parameters we estimate Neel temperatures for both spin structures within the molecular field approximation and show τ₁ (plaquettes) spin configuration to be more favorable than τ₂ (zigzags).     

First-principle calculation for the phonon structure on iron-based superconductors

We perform first-principle phonon calculations for three typical iron-based superconductors, i.e., LaFeAsO,BaFe₂As₂, and FeSe. Though those crystals have different structures, we find that the optical modes associated with Fe vibration have almost similar characters. Moreover, we examine the pressure effect on phonons in FeSe. By increasing the external pressure, the phonon mode frequency related to Fe vibration effectively rises up and the electronic density of states at Fermi level also increases. These results may correlate to the critical temperature enhancement under high pressure.     

The magnetism for NN AFM ground state in Fe-based superconductor: Sr1−xKxFe2As2

The crystal structure, magnetism properties, and density of states for FeAs layered compound SrFe₂As₂ have been investigated by using the density functional theory (DFT) method. The magnetism under a checkerboard nearest neighbor anti-ferromagnetic (NN AFM) and ferromagnetic (FM) order ground-state have been analyzed with substitution for Sr with K ion in Sr_1−xK_xFe₂As₂. The results indicate that the distortion of FeAs tetrahedrons is sensitive to the electron doping concentration. The system magnetism was suppressed by K doping in NN-AFM ground state instead of FM. The density of states at Fermi level N(E_F) under NN AFM ground state would be regarded as a driving force for the increased T_c of Sr_1−xK_xFe₂As₂ system as observed experimentally. Our calculation reflects that NN AFM type spin fluctuation may still exist in the Sr_1−xK_xFe₂As₂ system and it may be an origin of strong spin fluctuation in this system besides the spin density wave (SDW) states.     

Effect of the distortion of FeX4 (X = P,As) tetrahedron for the electronic structure of iron-pnictide system

We have performed an ab initio band structure calculation for the new high-T_c related iron-pnictide compounds LaFeXO (X = P, As), BaFe₂As₂, CaFe₂As₂ and LiFeAs (X = P, As). We found that LaFeXO and CaFe₂As₂ have many similarities in their band structures, which is expected by an ionic model. We found that the degree of distortion of FeAs₄ tetrahedra in LaFeAsO considerably changes the slope of the density of states near the Fermi level, and this result may explain why REFeAsO (RE = Nd, Sm, …) have higher T_c than LaFeAsO when electrons are doped. For all the above compounds, the density of states at the Fermi level decreases when X atoms approaches to the Fe–Fe plane, which means that the hybridization between Fe and X orbitals considerably expands the Fe d-bands.     

Electronic structures of doped BaFe<Subscript>2</Subscript>As<Subscript>2</Subscript> materials: virtual crystal approximation versus super-cell approach

Using virtual crystal approximation and super-cell methods for doping, a detailedcomparative study of electronic structures of various doped BaFe₂As₂ materials by first principlessimulations is presented. Electronic structures remain unaltered for both the methods incase of passive site doping but in case of active site doping, the electronic structurefor virtual crystal approximation method differ from that of the super-cell methodspecially in the higher doping concentrations. For example, both of these methods giverise to a similar density of states and band structures in case of hole doping (replacingK in place of Ba) and isovalent P doping on As site. But in case of electron doped (Co inplace of Fe) systems with higher doping concentration, electronic structures calculatedusing virtual crystal approximation approach deviates from that of the super-cell method.On the other hand, in case of low isovalent Ru doping at the Fe site implemented byvirtual crystal approximation, one acquires an extra shift in the chemical potential incomparison to that for the super-cell method. This shift may be utilized to predict thecorrect electronic structure as well as the calculated Fermi surfaces within virtualcrystal approximation. But for higher Ru (that has different electronic configuration thanFe) doping concentration, simple shifting of chemical potential fails, the calculatedelectronic structure via virtual crystal approximation approach is very different fromthat by the super-cell formalism.