Iron Chalcogenide Superconductors Research Articles

Vortex pinning properties in Fe-chalcogenides

Among the families of iron-based superconductors, the 11-family is one of the most attractive for high field applications at low temperatures. Optimization of the fabrication processes for bulk, crystalline and/or thin film samples is the first step in producing wires and/or tapes for practical high power conductors. Here we present the results of a comparative study of pinning properties in iron-chalcogenides, investigating the flux pinning mechanisms in optimized Fe(SeTex) and FeSe samples by current–voltage characterization, magneto-resistance and magnetization measurements. In particular, from Arrhenius plots in magnetic fields up to 9 T, the activation energy is derived as a function of the magnetic field, whereas the activation energy as a function of temperature, is derived from relaxation magnetization curves. The high pinning energies, high upper critical field versus temperature slopes near critical temperatures, and highly isotropic pinning properties make iron-chalcogenide superconductors a technological material which could be a real competitor to cuprate high temperature superconductors for high field applications.

Possible mixed coupling mechanism in FeTe1−xSex within a multiband Eliashberg approach

We show that the phenomenology of the iron chalcogenide superconductor FeTe1−xSex can be explained within an effective three-band -wave Eliashberg model. In particular, various experimental data reported in literature—the critical temperature, the energy gaps, the upper critical field, the superfluid density—can be reproduced by this model in a moderate strong-coupling regime provided that both an intraband phononic term and an interband antiferromagnetic spin-fluctuations term are included in the coupling matrix. The intraband coupling is unusual in Fe-based compounds and is required to explain the somehow anomalous association between gap amplitudes and Fermi surfaces, already evidenced by ARPES.

Evidence for orbital order and its relation to superconductivity in FeSe0.4Te0.6.

The emergence of nematic electronic states accompanied by a structural phase transition is a recurring theme in many correlated electron materials, including the high-temperature copper oxide- and iron-based superconductors. We provide evidence for nematic electronic states in the iron-chalcogenide superconductor FeSe0.4Te0.6 from quasi-particle scattering detected in spectroscopic maps. The symmetry-breaking states persist above T c into the normal state. We interpret the scattering patterns by comparison with quasi-particle interference patterns obtained from a tight-binding model, accounting for orbital ordering. The relation to superconductivity and the influence on the coherence length are discussed.

Magnetic and magnetotransport studies of iron-chalcogenide superconductor Fe(Se0.4Te0.6)0.82: observation of thermally activated transport and flux jump

The magnetic and magneto-transport behavior of the Fe-based superconductor of nominal composition Fe(Se0.4Te0.6)0.82 has been investigated. Different superconducting parameters such as critical fields, coherence length, penetration depth and the Ginzburg–Landau parameter (κ) have been estimated for the present compound. The large value of κ (∼253) is in line with the unconventional type-II nature of the studied superconductor. Thermally activated transport behavior in the presence of an external magnetic field across the superconducting transition region indicates a crossover from a single-vortex pinning regime to a collective flux creep regime at 50 kOe. The sample shows anomalous field dependence of flux flow resistance, which is presumably connected to the inherent superconducting state of the sample. The isothermal resistivity data as a function of external magnetic field show a signature of flux jump below the superconducting transition temperature (Tc). The effect of hydrostatic pressure on the superconducting properties of the compound has also been investigated and about 3 K shift in Tc has been observed with the application of 10 kbar of pressure.

Effect of magnetic frustration on nematicity and superconductivity in iron chalcogenides

Over the past few years Fe chalcogenides (FeSe/Te) have advanced to the forefront of Fe-based superconductors (FeBS) research. The most intriguing results thus far are for intercalated and monolayer FeSe, however experimental studies are still inconclusive. Yet, bulk FeSe itself remains an unusual case when compared with pnictogen-based FeBS, and may hold clues to understanding the more exotic FeSe-derivatives. The FeSe phase diagram is unlike the pnictides: the orthorhombic distortion, which is likely to be of a "spin-nematic" nature in numerous pnictides, is not accompanied by magnetic order in FeSe, and the superconducting transition temperature $T_{c}$ rises significantly with pressure before decreasing. In this paper we show that the magnetic interactions in chalcogenides, as opposed to pnictides, demonstrate unusual (and unanticipated) frustration, which suppresses magnetic, but not nematic order, favors ferro-orbital order in the nematic phase and can naturally explain the nonmonotonic pressure dependence of the superconducting critical temperature $T_{c}(P)$.

Spin-liquid polymorphism in a correlated electron system on the threshold of superconductivity

We report neutron scattering measurements which reveal spin-liquid polymorphism in an "11" iron chalcogenide superconductor. It occurs when a poorly metallic magnetic state of FeTe is tuned toward superconductivity by substitution of a small amount of tellurium with isoelectronic sulfur. We observe a liquid-like magnetic response, which is described by the coexistence of two disordered magnetic phases with different local structures whose relative abundance depends on temperature. One is the ferromagnetic (FM) plaquette phase observed in undoped, nonsuperconducting FeTe, which preserves the C4 symmetry of the underlying square lattice and is favored at high temperatures, whereas the other is the antiferromagnetic plaquette phase with broken C4 symmetry, which emerges with doping and is predominant at low temperatures. These findings suggest the coexistence of and competition between two distinct liquid states, and a liquid-liquid phase transformation between these states, in the electronic spin system of FeTe(1-x)(S,Se)(x). We have thus discovered the remarkable physics of competing spin-liquid polymorphs in a correlated electron system approaching superconductivity. Our results facilitate an understanding of large swaths of recent experimental data in unconventional superconductors. In particular, the phase with lower C2 local symmetry, whose emergence precedes superconductivity, naturally accounts for a propensity for forming electronic nematic states which have been observed experimentally, in cuprate and iron-based superconductors alike.

Observation of universal strong orbital-dependent correlation effects in iron chalcogenides.

Establishing the appropriate theoretical framework for unconventional superconductivity in the iron-based materials requires correct understanding of both the electron correlation strength and the role of Fermi surfaces. This fundamental issue becomes especially relevant with the discovery of the iron chalcogenide superconductors. Here, we use angle-resolved photoemission spectroscopy to measure three representative iron chalcogenides, FeTe0.56Se0.44, monolayer FeSe grown on SrTiO3 and K0.76Fe1.72Se2. We show that these superconductors are all strongly correlated, with an orbital-selective strong renormalization in the dxy bands despite having drastically different Fermi surface topologies. Furthermore, raising temperature brings all three compounds from a metallic state to a phase where the dxy orbital loses all spectral weight while other orbitals remain itinerant. These observations establish that iron chalcogenides display universal orbital-selective strong correlations that are insensitive to the Fermi surface topology, and are close to an orbital-selective Mott phase, hence placing strong constraints for theoretical understanding of iron-based superconductors.

FeTe0.55Se0.45: A multiband superconductor in the clean and dirty limit

The detailed optical properties of the multiband iron-chalcogenide superconductor FeTe$_{0.55}$Se$_{0.45}$ have been reexamined for a large number of temperatures above and below the critical temperature $T_c=14$ K for light polarized in the a-b planes. Instead of the simple Drude model that assumes a single band, above $T_c$ the normal-state optical properties are best described by the two-Drude model that considers two separate electronic subsystems; we observe a weak response ($\omega_{p,D;1}\simeq 3000$ cm$^{-1}$) where the scattering rate has a strong temperature dependence ($1/\tau_{D,1}\simeq 32$ cm$^{-1}$ for $T \gtrsim T_c$), and a strong response ($\omega_{p,D;2}\simeq 14\,500$ cm$^{-1}$) with a large scattering rate ($1/\tau_{D,2}\simeq 1720$ cm$^{-1}$) that is essentially temperature independent. The multiband nature of this material precludes the use of the popular generalized-Drude approach commonly applied to single-band materials, implying that any structure observed in the frequency dependent scattering rate $1/\tau(\omega)$ is spurious and it cannot be used as the foundation for optical inversion techniques to determine an electron-boson spectral function $\alpha^2 F(\omega)$. Below $T_c$ the optical conductivity is best described using two superconducting optical gaps of $2\Delta_1\simeq 45$ and $2\Delta_2 \simeq 90$ cm$^{-1}$ applied to the strong and weak responses, respectively. The scattering rates for these two bands are vastly different at low temperature, placing this material simultaneously in both clean and dirty limit. Interestingly, this material falls on the universal scaling line initially observed for the cuprate superconductors.

Crossover from hole- to electron-dominant regions in iron-chalcogenide superconductors induced by Te/Se substitution

We have investigated a Te/Se substitution effect on the field dependence of Hall resistivity in FeSe1−xTex (x = 0.5–0.7) thin films grown on LaAlO3 and CaF2 substrates. By observing the magnetic field dependence of Hall resistivity, the crossover from hole- to electron-dominant regions is observed to occur between x = 0.5 and 0.6 in the films on LaAlO3, while no such crossover is observed in those on CaF2. The results indicate that the substitution of Te for Se effectively acts as electron doping, while the lattice strain also has an additional effect on the balance of hole and electron densities. These two factors can be independently used to optimize superconducting transition temperature so as to tune the doping level near the boundary where the hole density becomes equal to the electron density.

QSGW+DMFT: an electronic structure scheme for the iron pnictides and beyond

While in strongly correlated materials one often focuses on local electronic correlations, the influence of non-local exchange and correlation effects beyond band-theory can be pertinent in systems with more extended orbitals. Thus in many compounds an adequate theoretical description requires the joint treatment of local and non-local self-energies. Here, I will argue that this is the case for the iron pnictide and chalcogenide superconductors. As an approach to tackle their electronic structure, I will detail the implementation of the recently proposed scheme that combines the quasi-particle self-consistent GW approach with dynamical mean-field theory: QSGW+DMFT. I will showcase the possibilities of QSGW+DMFT with an application on BaFe2As2. Further, I will discuss the empirical finding that in pnictides dynamical and non-local correlation effects separate within the quasi-particle band-width.

Strain effects in monolayer iron-chalcogenide superconductors

Successful fabrication of one monolayer FeSe on SrTiO3 represented a real breakthrough in searching for high-Tc Fe-based superconductors ([]). Motivated by this important discovery, we studied the effects of tensile strain on one monolayer and bulk iron-chalcogenide superconductors (FeSe and FeTe), showing that it produces important magnetic and electronic changes in the systems. We found that the magnetic ground state of bulk and monolayer FeSe is the block-checkerboard phase, which turns into the collinear stripe phase under in-plane tensile strain. FeTe, in both bulk and monolayer phases, shows two magnetic transitions upon increasing the tensile strain: from bicollinear in the ground state to block-checkerboard ending up to the collinear antiferromagnetic phase which could bring it in the superconducting state. Finally, the study of the mechanical properties of both FeSe and FeTe monolayers reveals their enormous tensile strain limits and opens the possibility to grow them on different substrates.

Electronic structure of ruthenium-doped iron chalcogenides

The structural and electronic properties of hypothetical RuxFe1−xSe and RuxFe1−xTe systems have been investigated from first principles within the density functional theory (DFT). Reasonable values of lattice parameters and chalcogen atomic positions in the tetragonal unit cell of iron chalcogenides have been obtained with the use of norm-conserving pseudopotentials. The well known discrepancies between experimental data and DFT-calculated results for structural parameters of iron chalcogenides are related to the semicore atomic states which were frozen in the used here approach. Such an approach yields valid results of the electronic structures of the investigated compounds. The Ru-based chalcogenides exhibit the same topology of the Fermi surface (FS) as that of FeSe, differing only in subtle FS nesting features. Our calculations predict that the ground states of RuSe and RuTe are nonmagnetic, whereas those of the solid solutions RuxFe1−xSe and RuxFe1−xTe become the single- and double-stripe antiferromagnetic, respectively. However, the calculated stabilization energy values are comparable for each system. The phase transitions between these magnetic arrangements may be induced by slight changes of the chalcogen atom positions and the lattice parameters a in the unit cell of iron selenides and tellurides. Since the superconductivity in iron chalcogenides is believed to be mediated by the spin fluctuations in single-stripe magnetic phase, the RuxFe1−xSe and RuxFe1−xTe systems are good candidates for new superconducting iron-based materials.

Intrinsic anisotropy of the superconductivity in FeSe1-xTex (x = 0.6) observed by specific heat in magnetic fields

Low-temperature specific heat measurements in various magnetic fields parallel and perpendicular to the c-axis for annealed single crystals of the iron-chalcogenide superconductor FeSe1-xTex have revealed that the anisotropy of the enhancement of the residual electronic- specific-heat-coefficient in the ground state by the application of magnetic field, namely, the anisotropy of the upper critical field, Hc2, is 2.2 for x = 0.6, which is different from the anisotropy of Hc2 estimated from the resistivity measurements in non-annealed single crystals of x = 0.6 [Khim et al. 2010 Phys. Rev. B 81 184511]. It appears that the anisotropy of Hc2 strongly depends on the content of excess iron included in a crystal.

Emergence of magnetism and controlling factors of superconductivity in Li/Na-ammonia cointercalatedFeSe1−zTez

The discovery of superconductivity in alkali-ammonia co-intercalated FeSe has generated intensive interest because of their highest Tc (~ 45 K) among iron-chalcogenide superconductors with bulk form. Here, we report the phase diagrams of two series of Li/Na-ammonia co-intercalated FeSe1-zTez. When superconductivity is suppressed by Te doping, the magnetic ordering states are emergent. Moreover, a novel phase Lix(NH3)yFe2-{\delta}Te2 with possible antiferromagnetism is discovered. This strongly indicates the intimate relation between superconductivity and magnetism in these materials, like in other iron-based superconductors. On the other hand, comparative structure analysis with FeSe1-zTez suggests that although there is remarkable similarity in phase diagrams for both iron-chalcogenide and iron-pnictide superconductors, the different types of anions with different charges lead to the dissimilar controlling factors in superconductivity for both classes of materials. This opens up an opportunity to tune the superconductivity in iron-chalcogenide superconductors in more ways than just one.

Unabridged phase diagram for single-phased FeSexTe1-x thin films

A complete phase diagram and its corresponding physical properties are essential prerequisites to understand the underlying mechanism of iron-based superconductivity. For the structurally simplest 11 (FeSeTe) system, earlier attempts using bulk samples have not been able to do so due to the fabrication difficulties. Here, thin FeSexTe1-x films with the Se content covering the full range (0 ≤ x ≤ 1) were fabricated by using pulsed laser deposition method. Crystal structure analysis shows that all films retain the tetragonal structure in room temperature. Significantly, the highest superconducting transition temperature (TC = 20 K) occurs in the newly discovered domain, i.e., 0.6 ≤ x ≤ 0.8. The single-phased superconducting dome for the full Se doping range is the first of its kind in iron chalcogenide superconductors. Our results present a new avenue to explore novel physics as well as to optimize superconductors.

Effect of pressure-driven local structural rearrangement on the superconducting properties ofFeSe0.5Te0.5

The pressure dependence of the superconducting transition temperature ${T}_{\mathrm{c}}$, the local structure, and the electronic properties of the iron chalcogenide superconductor ${\mathrm{FeSe}}_{0.5}{\mathrm{Te}}_{0.5}$ was investigated by means of SQUID magnetometry and site-selective polarized x-ray absorption spectroscopy at the iron and selenium $K$-edges. The measurements reveal a discontinuous decrease of the local bond distances by crossing a tetragonal to monoclinic structural phase transition at ${p}_{\mathrm{S}}\ensuremath{\sim}2.7$ GPa. The electronic structure, however, evolves evenly, but the superconducting properties are highly affected by changes in the local structure. These results underline the close connection of the lattice and the superconductivity in the iron-based superconductors.

Superconducting Gap and Symmetry in FeSe1−xTex Studied by Specific Heat in Magnetic Fields

In order to investigate details of the superconducting (SC) gap in the iron-chalcogenide superconductors, the specific heat, C, of FeSe_1-x_Te_x_ with x=0.6-1 has been measured in magnetic fields. Using the two-gap model, it has been found that the smaller SC gap is significantly depressed by the application of magnetic field, resulting in the increase of the slope of the C/T vs T^2^ plot at low temperatures. From the specific-heat measurements at very low temperatures down to 0.4 K, it has been found that the enhancement of the residual electronic-specific-heat-coefficient in the ground state, gamma_0_, by the application of magnetic field is much smaller than that expected for superconductors with the typical s-wave or d-wave SC paring symmetry, which is in sharp contrast to the significant enhancement of gamma_0 observed in the iron-pnictide superconductors. These results are discussed in relation to the multi-band effect in the iron-based superconductors.

Phase separation in AyFe2-xSe2(A= K, Rb, Cs) superconductors

The interplay between superconductivity, magnetism and crystal structure in iron-based superconductors has attracted a great interest in the recent years as it is considered to be the key for understanding the mechanisms responsible for high temperature superconductivity. Alkali metal intercalated iron chalcogenide superconductors (A122) exhibit unique behavior which is not observed in other iron-based superconducting materials such as antiferromagnetic ordering above room temperature and iron vacancies ordering. These materials have complex crystal structures with several phase transitions and are mixtures of phases even in the form usually described as a single crystal. A pronounced reversible phase separation revealed in A122 single crystals, as well as controversies regarding the origin of superconductivity and the stoichiometry and symmetry of the superconducting phase are still in the forefront of scientific activity. Here we will present a diffraction study of the crystal structures, antiferromagnetic ordering and intrinsic phase separation in alkali-metal iron chalcogenides [1]. The complementary scanning electron microscope study, including high-resolution electron back-scatter diffraction mapping will be also presented [2].

Electronic structure of Co-substituted FeSe superconductor probed by soft x-ray spectroscopy and density functional theory

We study the crystalline and electronic properties of the ${\text{Fe}}_{1\ensuremath{-}x}{\text{Co}}_{x}\text{Se}$ system ($x=0,0.25,0.5,0.75$, and 1.0) using x-ray diffraction, x-ray spectroscopy, and density functional theory. We show that the introduction of Co $3d$ states in FeSe relaxes the bond strengths and induces a structural transition from tetragonal to hexagonal whose crossover takes place at $x\ensuremath{\approx}0.38$. This structural transition in turn modifies the magnetic order, which can be related to the spin state. Using resonant inelastic x-ray scattering, we estimate the spin state of the system; FeSe is found to be in a high-spin state $(S=2)$, but Fe is reduced to a low-spin state upon Co substitution of $x\ensuremath{\le}0.25$, well below the structural transition. Finally, we show evidence that FeSe is a moderately correlated system but the introduction of Co into the host lattice weakens the correlation strength for $x\ensuremath{\ge}0.25$. These novel findings are important to unravel the mechanisms responsible for the superconducting state in iron-chalcogenide superconductors.

Unusual band renormalization in the simplest iron-based superconductorFeSe1−x

The electronic structure of the iron chalcogenide superconductor ${\text{FeSe}}_{1\ensuremath{-}x}$ was investigated by high-resolution angle-resolved photoemission spectroscopy (ARPES). The results were compared to DFT calculations showing some significant differences between the experimental electronic structure of ${\text{FeSe}}_{1\ensuremath{-}x}$, DFT calculations, and existing data on ${\text{FeSe}}_{x}{\text{Te}}_{1\ensuremath{-}x}$. The bands undergo a pronounced orbital-dependent renormalization, different from what was observed for ${\text{FeSe}}_{x}{\text{Te}}_{1\ensuremath{-}x}$ and any other pnictides.