Density functional studies of 26K superconducting LaFeAs(O,F) are reported. We find a low carrier density, high density of states, $N(E_F)$ and modest phonon frequencies relative to $T_c$. The high $N(E_F)$ leads to proximity to itinerant magnetism, with competing ferromagnetic and antiferromagnetic fluctuations and the balance between these controlled by doping level. Thus LaFeAs(O,F) is in a unique class of high $T_c$ superconductors: high $N(E_F)$ ionic metals near magnetism.
By a systematic study of the hydrogen-doped LaFeAsO system by means of dc resistivity, dc magnetometry, and muon-spin spectroscopy we addressed the question of universality of the phase diagram of rare-earth-1111 pnictides. In many respects, the behaviour of LaFeAsO_(1-x)H_(x) resembles that of its widely studied F-doped counterpart, with H^- realizing a similar (or better) electron-doping in the LaO planes. In a x = 0.01 sample we found a long-range SDW order with T_n = 119 K, while at x = 0.05 the SDW establishes only at 38 K and, below T_c = 10 K, it coexists at a nanoscopic scale with bulk…
The phonon dispersion was measured at room temperature along (0,0,L) in the tetragonal phase of LaFeAsO using inelastic x-ray scattering. Spin-polarized first-principles calculations imposing various types of antiferromagnetic order are in better agreement with the experimental results than nonmagnetic calculations, although the measurements were made well above the magnetic ordering temperature, T_N. Splitting observed between two A_{1g} phonon modes at 22 and 26 meV is only observed in spin-polarized calculations. Magneto-structural effects similar to those observed in the AFe_2As_2 material…
We describe the low temperature behaviour of the magnetic susceptibility of Cd2Re2O7 in terms of a Landau theory of structural phase transitions. We calculate the zero temperature Pauli susceptibility using a tight-binding approach to reveal the mechanism of coupling between the structural order parameter and itinerant magnetism.
We present $^{75}$As Nuclear Magnetic and Quadrupole Resonance results (NMR, NQR) on a new set of LaFeAsO$_{1-x}$F$_x$ polycrystalline samples. Improved synthesis conditions led to more homogenized samples with better control of the fluorine content. The structural$\equiv$nematic, magnetic, and superconducting transition temperatures have been determined by NMR spin-lattice relaxation rate and AC susceptibility measurements. The so-determined phase diagram deviates from the published one especially for low F-doping concentrations. However, if the doping level is determined from the NQR spectra…
Theoretical calculations are performed to understand the electronic structure and magnetic properties of CuFe$_2$Ge$_2$. The band structure reveal large electron density $N(E_F)$ at the Fermi level suggesting strong itinerant character of magnetism. The Fermi surface is dominated by two dimensional sheet like structures, with potentially strong nesting between them. The magnetic ground state appears to be ferromagnetic along $a$ and antiferromagnetic in other directions. The results show that CuFe$_2$Ge$_2$ is an antiferromagnetic metal, with similarities to the Fe-based superconductors; such …
To examine the role of magnetism in superconductivity of iron-based superconductors, we first present first-principles optical calculations on three representative parent compounds: LaFeAsO, BaFe2As2 and LiFeAs. Both nonmagnetic (NM) and spin-density wave (SDW) with striped antiferromagnetic order are considered. Due to their layer structure, these compounds in NM states show anomalously large optical anisotropy with a conductivity ratio $σ_{zz}/σ{xx}$ as large as 313% in LaFeAsO and 530% in LiFeAs. Interestingly the giant optical anisotropy is significantly suppressed by SDW. On the other han…
We have studied the interplay of magnetism and superconductivity in LaFeAsO$_{1-x}$F$_x$ and Ca(Fe$_{1-x}$Co$_x$)$_2$As$_2$. While antiferromagnetic spin density wave formation is suppressed and superconductivity evolves, all samples show a doping independent strong increase of the normal state susceptibility upon heating which appears a general feature of iron pnictides. The data provide evidence for robust local antiferromagnetic correlations persisting even in the superconducting regime of the phase diagram.
The electronic structure and magnetism of LiFeO$_{2}$Fe$_{2}$Se$_{2}$ are investigated using the first-principle calculations. The ground state is N$\acute{e}$el antiferromagnetic (AFM) Mott insulating state for Fe1 with localized magnetism in LiFeO$_{2}$ layer and striped AFM metallic state for Fe2 with itinerant magnetism in Fe$_{2}$Se$_{2}$ layer, accompanied with a weak interlayer AFM coupling between Fe1 and Fe2 ions, resulting in a coexistence of localized and itinerant magnetism. Moreover, the layered LiFeO$_{2}$ is found to be more than an insulating block layer but responsible for enh…
High temperature superconductivity is often found in the vicinity of antiferromagnetism. This is also true in LaFeAsO$_{1-x}$F$_{x}$ ($x \leq$ 0.2) and many other iron-based superconductors, which leads to proposals that superconductivity is mediated by fluctuations associated with the nearby magnetism. Here we report the discovery of a new superconductivity dome without low-energy magnetic fluctuations in LaFeAsO$_{1-x}$F$_{x}$ with 0.25$\leq x \leq$0.75, where the maximal critical temperature $T_c$ at $x_{opt}$ = 0.5$\sim$0.55 is even higher than that at $x \leq$ 0.2. By nuclear magnetic res…
The interplay between magnetism and superconductivity in LaFeAsO_0.945F_0.055 was studied as a function of hydrostatic pressure up to p~2.4GPa by means of muon-spin rotation (\muSR) and magnetization measurements. The application of pressure leads to a substantial decrease of the magnetic ordering temperature T_N and a reduction of the magnetic phase volume and, at the same time, to a strong increase of the superconducting transition temperature T_c and the diamagnetic susceptibility. From the volume sensitive \muSR measurements it can be concluded that the superconducting and the magnetic are…
We used the proximity effect as a tool to achieve an ideal (barrier - free) NS boundary for quantitative evaluation of transport phenomena that accompany converting dissipative current into supercurrent in NS systems with unconventional superconductors, single - crystal chalcogenide FeSe and granulated pnictide LaO(F)FeAs. Using features (limitations) of Andreev reflection in the NS systems with dispersion of the electron spin subbands, we revealed direct evidence for spin - polarized nature of transport and the absence of residual magnetization in iron - based superconductors in the normal st…
A Kondo-lattice theory is applied to the crossover between local-moment magnetism for almost half fillings of electrons and itinerant-electron magnetism away from the half filling. In clean systems with no disorder, the bandwidth W^* of quasiparticles is non-zero and of the order of |J| at T=0K even in the limit of the half filling, with J the superexchange interaction constant between nearest neighbors. The so called Gutzwiller's term also contributes to W^* away from the half filling; it is approximately proportional to doping concentrations measured from the half filling. Magnetism is enhan…
The duality between localized and itinerant nature of magnetism in $5\textit{f}$ electron systems has been a longstanding puzzle. Here, we report inelastic neutron scattering measurements, which reveal both local and itinerant aspects of magnetism in a single crystalline system of UPt$_{2}$Si$_{2}$. In the antiferromagnetic state, we observe broad continuum of diffuse magnetic scattering with a resonance-like gap of $\approx$ 7 meV, and surprising absence of coherent spin-waves, suggestive of itinerant magnetism. While the gap closes above the Neel temperature, strong dynamic spin correlations…
We present the magnetic structure of the itinerant monoarsenide, FeAs, with the B31 structure. Powder neutron diffraction confirms incommensurate modulated magnetism with wavevector $\mathbf{q} = (0.395\pm0.001)\mathbf{c}^*$ at 4 K, but cannot distinguish between a simple spiral and a collinear spin-density wave structure. Polarized single crystal diffraction confirms that the structure is best described as a non-collinear spin-density wave arising from a combination of itinerant and localized behavior with spin amplitude along the b-axis direction being (15 $\pm$ 5)% larger than in the a-dire…
We report on the magnetic behavior of oxygen deficient LaFeAsO1-x (x-0.10) compound, prepared by one-step synthesis, which crystallizes in the tetragonal (S.G. P4/nmm) structure at room temperature. Resistivity measurements show a strong anomaly near 150 K, which is ascribed to the spin density wave (SDW) instability. On the other hand, dc magnetization data shows paramagnetic-like features down to 5 K, with an effective moment of 0.83 mB/Fe. 57Fe Mossbauer studies (MS) have been performed at 95 and 200 K. The spectra at both temperatures are composed of two sub-spectra. At 200 K the major one…
Within the framework of density functional theory we investigate the nature of magnetism in various families of Fe-based superconductors. (i) We show that magnetization of stripe-type antiferromagnetic order always becomes stronger when As is substituted by Sb in LaOFeAs, BaFe$_2$As$_2$ and LiFeAs. By calculating Pauli susceptibilities, we attribute the magnetization increase obtained after replacing As by Sb to the enhancement of an instability at $(π,π)$. This points to a strong connection between Fermi surface nesting and magnetism, which supports the theory of the itinerant nature of magne…
Metallic ferromagnets with strongly interacting electrons often exhibit remarkable electronic phases such as ferromagnetic superconductivity, complex spin textures, and nontrivial topology. In this report, we discuss the synthesis of a layered magnetic metal NiTa$_4$Se$_8$ (or Ni$_{1/4}$TaSe$_{2}$) with a Curie temperature of 58 Kelvin. Magnetization data and \textit{ab initio} calculations indicate that the nickel atoms host uniaxial ferromagnetic order of about 0.7$μ_{B}$ per atom, while an even smaller moment is generated in the itinerant tantalum conduction electrons. Strong correlations a…
The electronic structure and magnetism of a new magnetic intercalation compound (Li0.8Fe0.2)OHFeSe are investigated theoretically. The electronic structure calculations predict that the Fe in the (Li,Fe)OH intercalated layer is in +2 valence state, i.e. there is electron doping to the FeSe layer, resulting in the shrinking of the Fermi surface (FS) pocket around Gamma and a strong suppression of dynamical spin susceptibility at M in comparison with the bulk FeSe compound. The ground state of the FeSe layer is a striped antiferromagnetic (SAFM) metal, while the (Li,Fe)OH layer displays a very w…
The layered iron superconductors are discussed using electronic structure calculations. The four families of compounds discovered so far, including Fe(Se,Te) have closely related electronic structures. The Fermi surface consists of disconnected hole and electron cylinders and additional hole sections that depend on the specific material. This places the materials in proximity to itinerant magnetism, both due to the high density of states and due to nesting. Comparison of density functional results and experiment provides strong evidence for itinerant spin fluctuations, which are discussed in r…
Neutron scattering measurements were performed to investigate magnetic excitations in a single-crystal sample of the ternary iron arsenide BaFe2As2, a parent compound of a recently discovered family of Fe-based superconductors. In the ordered state, we observe low energy spin-wave excitations with a gap energy of 9.8(4) meV. The in-plane spin-wave velocity v_ab and out-of-plane spin-wave velocity v_c measured at 12 meV are 280(150) and 57(7) meV A, respectively. At high energy, we observe anisotropic scattering centered at the antiferromagnetic wave vectors. This scattering indicates two-dimen…
Magnetism and nematic order are the two non-superconducting orders observed in iron-based superconductors. To elucidate the interplay between them and ultimately unveil the pairing mechanism, several models have been investigated. In models with quenched orbital degrees of freedom, magnetic fluctuations promote stripe magnetism which induces orbital order. In models with quenched spin degrees of freedom, charge fluctuations promote spontaneous orbital order which induces stripe magnetism. Here we develop an unbiased approach, in which we treat magnetic and orbital fluctuations on equal footing…
Identifying the nature of magnetism, itinerant or localized, remains a major challenge in condensed-matter science. Purely localized moments appear only in magnetic insulators, whereas itinerant moments more or less co-exist with localized moments in metallic compounds such as the doped-cuprate or the iron-based superconductors, hampering a thorough understanding of the role of magnetism in phenomena like superconductivity or magnetoresistance. Here we distinguish two antiferromagnetic modulations with respective propagation wave vectors of $Q_{\pm}$ = ($H \pm 0.557(1)$, 0, $L \pm 0.150(1)$) a…
We report on the crystal structure, physical properties, and electronic structure calculations for the ternary pnictide compound EuCr2As2. X-ray diffraction studies confirmed that EuCr2As2 crystalizes in the ThCr2Si2-type tetragonal structure (space group I4/mmm). The Eu ions are in a stable divalent state in this compound. Eu moments in EuCr2As2 order magnetically below Tm = 21 K. A sharp increase in the magnetic susceptibility below Tm and the positive value of the paramagnetic Curie temperature obtained from the Curie-Weiss fit suggest dominant ferromagnetic interactions. The heat capacity …
Quantum materials that feature magnetic long-range order often reveal complex phase diagrams when localized electrons become mobile. In many materials magnetism is rapidly suppressed as electronic charges dissolve into the conduction band. In materials where magnetism persists, it is unclear how the magnetic properties are affected. Here we study the evolution of the magnetic structure in Nd(1-x)Ce(x)CoIn(5) from the localized to the highly itinerant limit. We observe two magnetic ground states inside a heavy-fermion phase that are detached from unconventional superconductivity. The presence o…
The response of superconductors to controlled introduction of point-like disorder is an important tool to probe their microscopic electronic collective behavior. In the case of iron-based superconductors (IBS), magnetic fluctuations presumably play an important role in inducing high temperature superconductivity. In some cases, these two seemingly incompatible orders coexist microscopically. Therefore, understanding how this unique coexistence state is affected by disorder can provide important information about the microscopic mechanisms involved. In one of the most studied pnictide family, h…
The surprising discovery of high-$T_c$ superconductivity in iron-based compounds has prompted an intensive investigation on the role of interaction and magnetism in the these materials. Based on the general features of multi-bands and intermediate coupling strengths, a phenomenological theory of coexisting itinerant and localized electrons has been proposed to describe the low-energy physics in iron-based superconductors. It provides a unified framework to understand magnetic, superconducting, and normal phases, subject to further microscopic justification and experimental verification.
Itinerant Nature of Spin-Density-Wave Order in Ruddlesden-Popper Nickelates
Beijing National Laboratory for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences（中国科学院物理研究所）；School of Physical Sciences, University of Chinese Academy of Sciences（中国科学院大学物理科学学院）
We report muon-spin relaxation measurements on SrFeAsF, which is the parent compound of a newly discovered iron-arsenic-fluoride based series of superconducting materials. We find that this material has very similar magnetic properties to LaFeAsO, such as separated magnetic and structural transitions (TN = 120 K, Ts = 175 K), contrasting with SrFe2As2 where they are coincident. The muon oscillation frequencies fall away very sharply at TN, which suggests that the magnetic exchange between the layers is weaker than in comparable oxypnictide compounds. This is consistent with our specific heat m…
By calculating orbitally resolved Pauli susceptibilities within maximally localized Wannier orbital basis transformed from first principles band structures, we find that magnetism in Fe$_{1+x}$Te still has its itinerant origin even without Fermi surface nesting, provided orbital modulation of particle-hole excitations are considered. This leads to strong magnetic instabilities at wave vector (0,$π$)/($π$,0) in d$_{xz}$/d$_{yz}$ orbitals that are responsible for the bicollinear antiferromagnetic state as extra electrons donated from excess Fe are considered. Magnetic exchange coupling between e…
Heterostructures made of itinerant ferromagnets and superconductors are studied. In contrast to most previous models, ferromagnetism is not enforced as an external Zeeman field but induced in a correlated single-band model (CSBM) that displays itinerant ferromagnetism as a mean-field ground state. This allows us to investigate the influence of an adjacent superconducting layer on the properties of the ferromagnet in a self-consistent Bogoliubov-de Gennes approach. The CSBM displays a variety features not present in the Zeeman exchange model that influence the behavior of order parameters close…
This paper explains the multi-orbital band structures and itinerant magnetism of the iron-pnictide and chalcogenides. We first describe the generic band structure of an isolated FeAs layer. Use of its Abelian glide-mirror group allows us to reduce the primitive cell to one FeAs unit. From density-functional theory, we generate the set of eight Fe $d$ and As $p$ localized Wannier functions for LaOFeAs and their tight-binding (TB) Hamiltonian, $h(k)$. We discuss the topology of the bands, i.e. allowed and avoided crossings, the origin of the d6 pseudogap, as well as the role of the As $p$ orbita…
Recent applications of Quantum Monte Carlo (QMC) technique to Fe-based superconductors opened a way to directly verify the applicability of the itinerant scenario for these systems. Fe-based superconductors undergo various instabilities upon lowering temperature (magnetism, superconductivity, nematicity/orbital order), and one can check whether the hierarchy of instabilities obtained within the itinerant approach is the same as in unbiased QMC simulations. In a recent paper [arXiv:1512:08523] the authors considered the simplest two-band model with interaction tailored to favor orbital order. T…
Nematicity and magnetism are two key features in Fe-based superconductors, and their interplay is one of the most important unsolved problems. In FeSe, the magnetic order is absent below the structural transition temperature $T_{str}=90$K, in stark contrast that the magnetism emerges slightly below $T_{str}$ in other families. To understand such amazing material dependence, we investigate the spin-fluctuation-mediated orbital order ($n_{xz}\neq n_{yz}$) by focusing on the orbital-spin interplay driven by the strong-coupling effect, called the vertex correction. This orbital-spin interplay is v…
In this review article we present a survey of unconventional superconductors and their coexistence behaviour with magnetism. We focus on Ce- and U-based heavy fermion superconductors, in addition we discuss the rare earth borocarbide and skutterudite superconductors. We show that heavy fermion behaviour in Ce- and U- compounds should be described differently. While the Kondo-lattice model with localised 4f-electrons is appropriate for Ce-compounds, dual models including localised and itinerant 5f-electrons are necessary for U-compounds. We demonostrate that this leads to consistent results for…
The presence of macroscopic phase separation into superconducting and magnetic phases in LaFeAsO$_{1-x}$F$_x$ (LFAOF) and CaFe$_{1-x}$Co$_x$AsF (CFCAF) is demonstrated by muon spin rotation (muSR) measurement across their phase boundaries ($x=0.06$ for LFAOF and $x=0.075$--0.15 for CFCAF). In LFAOF, both magnetism and superconductivity develop simultaneously below a common critical temperature, $T_m =~ T_c =~ 18$ K, where the magnetism is characterized by strong randomness. A similar, but more distinct segregation of these two phases is observed in CFCAF, where the magnetic phase retains $T_m$…
We report an investigation into the superconducting and magnetic properties of Fe_{1+y}Se_{x}Te_{1-x} single crystals by magnetic susceptibility, muon spin rotation, and neutron diffraction. We find three regimes of behavior in the phase diagram for 0\leq x\leq 0.5: (i) commensurate magnetic order for x< 0.1, (ii) bulk superconductivity for $x\lesssim 0.1$, and (iii) a range \sim 0.25\leq x\leq 0.45 in which superconductivity coexists with static incommensurate magnetic order. The results are qualitatively consistent with a two-band mean-field model in which itinerant magnetism and extended s-…
A theory of Kondo lattices is applied to the crossover between local-moment magnetism and itinerant-electron magnetism in the t-J model on a quasi-two dimensional lattice. The Kondo temperature T_K is defined as a characteristic temperature or energy scale of local quantum spin fluctuations. Magnetism with T_N >> T_K, where T_N is the N\eel temperature, is characterized as local-moment one, while magnetism with T_N << T_K is characterized as itinerant-electron one. The Kondo temperature, which also gives a measure of the strength of the quenching of magnetic moments, is renormalized by the Foc…
We focus on a broad class of tetragonal itinerant systems sharing a tendency towards the spontaneous formation of incommensurate magnetism with ordering wavevectors $\mathbf{Q}_{1,2}=(π-δ,0)/(0,π-δ)$ or $\mathbf{Q}_{1,2}=(π,δ)/(-δ,π)$. Employing a Landau approach, we obtain the generic magnetic phase diagram and identify the leading instabilities near the paramagnetic-magnetic transition. Nine distinct magnetic phases exist that either preserve or violate the assumed $C_4$-symmetry of the paramagnetic phase. These are single- and double-$\mathbf{Q}$ phases consisting of magnetic stripes, helic…
Recent discovery of high T_c superconductivity in Fe-based compounds may have opened a new pathway to the room temperature superconductivity. The new materials feature FeAs layers instead of the signature CuO_2 planes of much-studied cuprates. A model Hamiltonian describing FeAs layers is introduced, highlighting the crucial role of puckering of As atoms in promoting d-electron itinerancy and warding off large local-moment magnetism of Fe ions, the main enemy of superconductivity. Quantum many-particle effects in charge, spin and multiband channels are explored and a nesting-induced spin densi…
The influence of static magnetic correlations on the temperature-dependent superfluid density ρ_s(T) is calculated for d-wave superconductors. In self-consistent calculations, itinerant holes form incommensurate spin density waves (SDW) which coexist with superconductivity. In the clean limit, the density of states is gapped, and ρ_s(T << T_c) is exponentially activated. In inhomogeneously-doped cases, the SDW are disordered and both the density of states and ρ_s(T) obtain forms indistinguishable from those in dirty but pure d-wave superconductors, in accordance with experiments. We conclude t…
We performed spin-polarized density functional calculations of lanthanide-series (Ln) iron oxypnictides LnFeAsO (Ln=La, Ce, Pr, Nd, Sm, and Gd) with constrained Fe magnetic moments, finding that in-plane dxy and out-of-plane dyz orbital characters are preferred for small Fe magnetic moments. Comparison of LnFeAsO compounds shows that the antiferromagnetism (AFM) from the Fe dxy orbital is itinerantly driven by orbital-dependent Fermi-surface nesting while AFM from the Fe dyz orbital is driven by superexchange mechanism. The Fe magnetic moments of the two orbital characters show different coupl…
In the generic phase diagram of heavy fermion systems, tuning an external parameter such as hydrostatic or chemical pressure modifies the superconducting transition temperature. The superconducting phase forms a dome in the temperature-tuning parameter phase diagram, which is associated with a maximum of the superconducting pairing interaction. Proximity to antiferromagnetism suggests a relation between the disappearance of antiferromagnetic order and superconductivity. We combine muon spin rotation, neutron scattering, and x-ray absorption spectroscopy techniques to gain access to the magneti…
