Iron Chalcogenide Superconductors Research Articles

Unveiling the quasiparticle behaviour in the pressure-induced high-Tc phase of an iron-chalcogenide superconductor

Superconductivity of iron chalocogenides is strongly enhanced under applied pressure yet its underlying pairing mechanism remains elusive. Here, we present a quantum oscillations study up to 45 T in the high-Tc phase of tetragonal FeSe0.82S0.18 up to 22 kbar. Under applied pressure, the quasi-two-dimensional multi-band Fermi surface expands and the effective masses remain large, whereas the superconductivity displays a threefold enhancement. Comparing with chemical pressure tuning of FeSe1−xSx, the Fermi surface expands in a similar manner but the effective masses and Tc are suppressed. These differences may be attributed to the changes in the density of states influenced by the chalcogen height, which could promote stronger spin fluctuations pairing under pressure. Furthermore, our study also reveals unusual scattering and broadening of superconducting transitions in the high-pressure phase, indicating the presence of a complex pairing mechanism.

Properties and Applications of Iron-Chalcogenide Superconductors.

Iron-chalcogenide superconductors continue to captivate researchers due to their diverse crystalline structures and intriguing superconducting properties, positioning them as both a valuable platform for theoretical investigations and promising candidates for practical applications. This review begins with a comprehensive overview of the fabrication techniques employed for various iron-chalcogenide superconductors, accompanied by a summary of their phase diagrams. Subsequently, it delves into the upper critical field, anisotropy, and critical current density. Furthermore, it discusses the successful fabrication of meters-long coated conductors and explores their applications in superconducting radio-frequency cavities and coils. Finally, several prospective avenues for future research are proposed.

The origin of the large Tc\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$T_{\\mathrm{c}}$\\end{document} variation in FeSe thin films probed by dual-beam pulsed laser deposition

FeSe is one of the most enigmatic superconductors. Among the family of iron-based compounds, it has the simplest chemical makeup and structure, and yet it displays superconducting transition temperature (Tc\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$T_{\ ext{c}}$\\end{document}) spanning 0 to 15 K for thin films, while it is typically 8 K for single crystals. This large variation of Tc\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$T_{\ ext{c}}$\\end{document} within one family underscores a key challenge associated with understanding superconductivity in iron chalcogenides. Here, using a dual-beam pulsed laser deposition (PLD) approach, we have fabricated a unique lattice-constant gradient thin film of FeSe which has revealed a clear relationship between the atomic structure and the superconducting transition temperature for the first time. The dual-beam PLD that generates laser fluence gradient inside the plasma plume has resulted in a continuous variation in distribution of edge dislocations within a single film, and a precise correlation between the lattice constant and Tc\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$T_{\ ext{c}}$\\end{document} has been observed here, namely, Tc∝c−c0\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$T_{\ ext{c}} \\propto \\sqrt{c- c_{0}}$\\end{document}, where c is the c-axis lattice constant (and c0\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$c_{0}$\\end{document} is a constant). This explicit relation in conjunction with a theoretical investigation indicates that it is the shifting of the dxy\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$d_{\ ext{xy}}$\\end{document} orbital of Fe which plays a governing role in the interplay between nematicity and superconductivity in FeSe.

Pseudospin-triplet pairing in iron-chalcogenide superconductors

Understanding the pairing symmetry is a crucial theoretical aspect in the study of unconventional superconductivity for interpreting experimental results. Here we study superconductivity of electron systems with both spin and pseudospin-1/2 degrees of freedom. By solving linearized gap equations, we derive a weak coupling criterion for the even-parity spin-singlet pseudospin-triplet pairing. It can generally mix with the on-site s-wave pairing since both of them belong to the same symmetry representation (A1g) and their mixture could naturally give rise to anisotropic intra-band pairing gap functions with or without nodes. This may directly explain why some of the iron-chalcogenide superconductors are fully gapped (e.g. FeSe thin film) and some have nodes (e.g. LaFePO and LiFeP). We also find that the anisotropy of gap functions can be enhanced when the principal rotation symmetry is spontaneously broken in the normal state such as nematicity, and the energetic stabilization of pseudospin-triplet pairings indicates the coexistence of nematicity and superconductivity. This could be potentially applied to bulk FeSe, where gap anisotropy has been experimentally observed.

Resurgence of superconductivity and the role of dxy hole band in FeSe1−xTex

Iron-chalcogenide superconductors display rich phenomena caused by orbital-dependent band shifts and electronic correlations. Additionally, they are potential candidates for topological superconductivity due to the band inversion between the Fe d bands and the chalcogen pz band. Here we present a detailed study of the electronic structure of the nematic superconductors FeSe1−xTex (0 < x < 0.4) using angle-resolved photoemission spectroscopy to understand the role of orbital-dependent band shifts, electronic correlations and the chalcogen band. We assess the changes in the effective masses using a three-band low energy model, and the band renormalization via comparison with DFT band structure calculations. The effective masses decrease for all three-hole bands inside the nematic phase, followed by a strong increase for the band with dxy orbital character. Interestingly, this nearly-flat dxy band becomes more correlated as it shifts towards the Fermi level with increasing Te concentrations and as the second superconducting dome emerges. Our findings suggests that the dxy hole band, which is very sensitive to the chalcogen height, could be involved in promoting an additional pairing channel and increasing the density of states to stabilize the second superconducting dome in FeSe1−xTex. This simultaneous shift of the dxy hole band and enhanced superconductivity is in contrast with FeSe1−xSx.

Magnetic Field-Induced Spin Nematic Phase Up to Room Temperature in Epitaxial Antiferromagnetic FeTe Thin Films Grown by Molecular Beam Epitaxy.

Electronic nematicity, where strong correlations drive electrons to align in a way that lowers the crystal symmetry, is ubiquitous among unconventional superconductors. Understanding the interplay of such a nematic state with other electronic phases underpins the complex behavior of these materials and the potential for tuning their properties through external stimuli. Here, we report magnetic field-induced spin nematicity in a model system tetragonal FeTe, the parent compound of iron chalcogenide superconductors, which exhibits a bicollinear antiferromagnetic order. The studies were conducted on epitaxial FeTe thin films grown on SrTiO3(001) substrates by molecular beam epitaxy, where the bicollinear antiferromagnetic order was confirmed by in situ atomic resolution scanning tunneling microscopy imaging. A 2-fold anisotropy is observed in in-plane angle-dependent magnetoresistance measurements, indicative of magnetic field-induced nematicity. Such 2-fold anisotropy persists up to 300 K, well-above the bicollinear antiferromagnetic ordering temperature of 75 K, indicating a magnetic field-induced spin nematic phase up to room temperature in the antiferromagnet FeTe.

Two superconducting states with broken time-reversal symmetry in FeSe1-xSx.

Iron-chalcogenide superconductors FeSe1-xSx possess unique electronic properties such as nonmagnetic nematic order and its quantum critical point. The nature of superconductivity with such nematicity is important for understanding the mechanism of unconventional superconductivity. A recent theory suggested the possible emergence of a fundamentally new class of superconductivity with the so-called Bogoliubov Fermi surfaces (BFSs) in this system. However, such an ultranodal pair state requires broken time-reversal symmetry (TRS) in the superconducting state, which has not been observed experimentally. Here, we report muon spin relaxation (μSR) measurements in FeSe1-xSx superconductors for 0 ≤ x ≤ 0.22 covering both orthorhombic (nematic) and tetragonal phases. We find that the zero-field muon relaxation rate is enhanced below the superconducting transition temperature Tc for all compositions, indicating that the superconducting state breaks TRS both in the nematic and tetragonal phases. Moreover, the transverse-field μSR measurements reveal that the superfluid density shows an unexpected and substantial reduction in the tetragonal phase (x > 0.17). This implies that a significant fraction of electrons remain unpaired in the zero-temperature limit, which cannot be explained by the known unconventional superconducting states with point or line nodes. The TRS breaking and the suppressed superfluid density in the tetragonal phase, together with the reported enhanced zero-energy excitations, are consistent with the ultranodal pair state with BFSs. The present results reveal two different superconducting states with broken TRS separated by the nematic critical point in FeSe1-xSx, which calls for the theory of microscopic origins that account for the relation between nematicity and superconductivity.

Direct Observation of Quantum Anomalous Vortex in Fe(Se,Te)

Vortices are topological defects of type-II superconductors in an external magnetic field. In a similar fashion to a quantum anomalous Hall insulator, quantum anomalous vortex (QAV) spontaneously nucleates due to orbital-and-spin exchange interaction between vortex core states and magnetic impurity moment, breaking time-reversal symmetry (TRS) of the vortex without an external field. Here, we used scanning superconducting quantum interference device microscopy (sSQUID) to search for its signatures in iron-chalcogenide superconductor Fe(Se,Te). Under zero magnetic field, we found a stochastic distribution of isolated anomalous vortices and antivortices with flux quanta $\Phi_0$. By applying a small local magnetic field under the coil of the nano-SQUID device, we observed hysteretic flipping of the vortices reminiscent of the switching of ferromagnetic domains, suggesting locally broken-TRS. We further showed vectorial rotation of a flux line linking a paired vortex-antivortex with the local field. These unique properties of the anomalous vortices satisfied the defining criteria of QAV. Our observation suggests a quantum vortex phase with spontaneous broken-TRS in a high-temperature superconductor.

Ultrafast Melting of Superconductivity in an Iron-Based Superconductor

Optical pumping of an ``unconventional'' iron-chalcogenide superconductor leads to a metastable state in which superconductivity disappears on very fast timescales, possibly due to magnetic correlations triggered by the pumping.

Single-crystal growth and superconductivity in RbNi2Se2

We report the synthesis and characterization of RbNi$_2$Se$_2$, an analog of the iron chalcogenide superconductor Rb$_x$Fe$_2$Se$_2$, via transport, angle resolved photoemission spectroscopy, and density functional theory calculations. A superconducting transition at $T_{c}$ = 1.20 K is identified. In normal state, RbNi$_2$Se$_2$ shows paramagnetic and Fermi liquid behaviors. A large Sommerfeld coefficient yields a heavy effective electron mass of $m^{*}\approx6m_{e}$. In the superconducting state, zero-field electronic specific-heat data $C_{es}$ can be described by a two-gap BCS model, indicating that RbNi$_2$Se$_2$ is a multi-gap superconductor. Our density functional theory calculations and angle resolved photoemission spectroscopy measurements demonstrate that RbNi$_2$Se$_2$ exhibits relatively weak correlations and multi-band characteristics, consistent with the multi-gap superconductivity.

The superconductivity and transport properties in FeTe with S addition

In the past few years, iron chalcogenide compounds have attracted considerable attentions due to its unique superconductivity and simplest structure. Till now, many studies have been devoted to explore the superconductivity in iron chalcogenides, including FeSe, FeTe, FeS and their derivatives produced by intermediate doping. However, compared with FeSe, although the superconductivity in S doped FeTe has been widely studied, very few attempts have been reported on the transport properties for this material. Herein the evolution of the superconductivity and the Hall effect up to high S addition levels in FeTe1-xSx (0 ≤ x ≤ 0.5) were studied. It suggests that S substitution for Te sites can effectively suppress the antiferromagnetic ordering and introduce bulk superconductivity in FeTe. The highest Tc ∼9.0 K is achieved in FeTe0.8S0.2 with nominal S content. Hall effect suggests that S addition in FeTe undergoes a reconstruction of hole-type Fermi surface, indicating doping or enhancement of scattering of hole carriers. This work systemically studied the superconductivity of FeTe with S addition and proposes complementary understanding for the intrinsic transport mechanism of iron-based superconductivity.

Phonon mechanism explanation of the superconductivity dichotomy between FeSe and FeS monolayers on SrTiO3 and other substrates

It was observed recently (K. Shigekawa et al, PNAS 116, 2470 (2019)) that while monolayer iron chalcigenide FeSe on SrTiO3 (STO) substrate has a very high critical temperature, its chemical and structural "twin" material FeS=STO has a very low Tc if any. To explain this the substrate interfacial phonon model of superconductivity in iron chalcogenides is further developed. The main glue is the oxygen ion (60mev) vibrations longitudinal optical (LO) mode. The mode propagates mainly in the TiO2 layer adjacent to the monolayer (and genrally present also in similar highly polarized ionic crystals like BaTiO3; rutile, anatase). It has stronger electron - phonon coupling to electron gas in FeSe than a well known (100mev) harder LO mode. It is shown that while (taking into account screened Coulomb repulsion efects) the critical temperature of FeSe on STO and TiO2 is above 65K, it becomes less than 5K for FeS due to two factors suppressing the electron - phonon coupling. The efective mass in the later is twice smaller and in addition the distance between the electron gas in FeSe to the vibrating substrate oxygen atoms is 15% smaller than in FeS reducinng the central peak in electron-phonon interaction. The theory is extended to other ionic insulating substrates.

Excess-iron driven spin glass phase in Fe1 + y Te1 – x Se x * *The work at Beijing Normal University is supported by the National Natural Science Foundation of China (Grant Nos. 11734002 and 11922402, X.L.). Work at Rice is supported by the US Department of Energy (DOE), Basic Energy Sciences (BES), under Contract No. DE-SC0012311 (P.D.). A portion

The iron-chalcogenide superconductor FeTe1–x Se x displays a variety of exotic features distinct from iron pnictides. Although much effort has been devoted to understanding the interplay between magnetism and superconductivity near x = 0.5, the existence of a spin glass phase with short-range magnetic order in the doping range (x ∼ 0.1–0.3) has rarely been studied. Here, we use DC/AC magnetization and (quasi) elastic neutron scattering to confirm the spin-glass nature of the short-range magnetic order in a Fe1.07Te0.8Se0.2 sample. The AC-frequency dependent spin-freezing temperature T f generates a frequency sensitivity ΔT f(ω)/[T f(ω)Δlog10 ω] ≈ 0.028 and the description of the critical slowing down with τ = τ 0(T f/T SG – 1)−z v gives T SG ≈ 22 K and zv ≈ 10, comparable to that of a classical spin-glass system. We have also extended the frequency-dependent T f to the smaller time scale using energy-resolution-dependent neutron diffraction measurements, in which the T N of the short-range magnetic order increases systematically with increasing energy resolution. By removing the excess iron through annealing in oxygen, the spin-freezing behavior disappears, and bulk superconductivity is realized. Thus, the excess Fe is the driving force for the formation of the spin-glass phase detrimental to bulk superconductivity.

Sulfur-induced magnetism in FeSe1−xSx thin films on LaAlO3 revealed by muon spin rotation/relaxation

Muon spin rotation/relaxation measurements were performed to investigate magnetic properties of FeSe$_{1-x}$S$_x$ thin films on LaAlO$_3$. A drastic decrease of the initial asymmetry was observed together with the peak structure in the temperature dependence of the relaxation rate of muon spins almost at the same temperature where kink anomalies were observed in the temperature dependent resistivity. With increasing S content, the anomaly temperature increased and the magnetic fluctuations at the lowest temperature were suppressed. These results show that the S substitution induces magnetism at low temperatures in FeSe$_{1-x}$S$_x$ thin films. Although the behaviors of the magnetic and nematic phases in FeSe films towards chemical pressure by S substitution are similar to those for bulk FeSe towards hydrostatic pressure, the behavior of $T_{\mathrm c}$ is significantly different between these systems. Our results demonstrate that the detailed comparative investigation among physical and chemical pressure effects is essentially important to understand the interplay of the magnetism, the nematicity and the superconductivity in iron chalcogenides.

A new Majorana platform in an Fe-As bilayer superconductor

Iron-chalcogenide superconductors have emerged as a promising Majorana platform for topological quantum computation. By combining topological band and superconductivity in a single material, they provide significant advantage to realize isolated Majorana zero modes. However, iron-chalcogenide superconductors, especially Fe(Te,Se), suffer from strong inhomogeneity which may hamper their practical application. In addition, some iron-pnictide superconductors have been demonstrated to have topological surface states, yet no Majorana zero mode has been observed inside their vortices, raising a question of universality about this new Majorana platform. In this work, through angle-resolved photoemission spectroscopy and scanning tunneling microscopy/spectroscopy measurement, we identify Dirac surface states and Majorana zero modes, respectively, for the first time in an iron-pnictide superconductor, CaKFe4As4. More strikingly, the multiple vortex bound states with integer-quantization sequences can be accurately reproduced by our model calculation, firmly establishing Majorana nature of the zero mode.

Canted antiferromagnetism in the quasi-one-dimensional iron chalcogenide BaFe2Se4

We report the synthesis and physical properties studies of quais-1D iron chalcogenide $\rm BaFe_2Se_4$ which shares the $\rm FeSe_4$ tetrahedra building motif commonly seen in the iron chalcogenide superconductors. A high-quality polycrystalline sample was achieved by solid-state reaction method and characterized by X-ray diffraction, electrical resistivity, magnetic susceptibility and neutron diffraction measurements. $\rm BaFe_2Se_4$ is a narrow gap semiconductor that magnetically orders at $\sim$ 310 K. Both neutron powder diffraction results and isothermal M-H loops suggest a canted antiferromagnetic structure where Fe sublattice are antiferromagnetically ordered along the c-axis quasi-1D chain direction, resulting in a net ferromagnetic moment in the perpendicular direction along the a-axis with tilted angle of 18.7$^\circ$ towards the b-axis.

Observation of robust edge superconductivity in Fe(Se,Te) under strong magnetic perturbation

The iron-chalcogenide high temperature superconductor Fe(Se,Te) (FST) has been reported to exhibit complex magnetic ordering and nontrivial band topology which may lead to novel superconducting phenomena. However, the recent studies have so far been largely concentrated on its band and spin structures while its mesoscopic electronic and magnetic response, crucial for future device applications, has not been explored experimentally. Here, we used scanning superconducting quantum interference device microscopy for its sensitivity to both local diamagnetic susceptibility and current distribution in order to image the superfluid density and supercurrent in FST. We found that in FST with 10% interstitial Fe, whose magnetic structure was heavily disrupted, bulk superconductivity was significantly suppressed whereas edge still preserved strong superconducting diamagnetism. The edge dominantly carried supercurrent despite of a very long magnetic penetration depth. The temperature dependences of the superfluid density and supercurrent distribution were distinctively different between the edge and the bulk. Our Heisenberg modeling showed that magnetic dopants stabilize anti-ferromagnetic spin correlation along the edge, which may contribute towards its robust superconductivity. Our observations hold implication for FST as potential platforms for topological quantum computation and superconducting spintronics.

On the Remarkable Superconductivity of FeSe and Its Close Cousins

Emergent electronic phenomena in iron-based superconductors have been at the forefront of condensed matter physics for more than a decade. Much has been learned about the origins and intertwined roles of ordered phases, including nematicity, magnetism, and superconductivity, in this fascinating class of materials. In recent years, focus has been centered on the peculiar and highly unusual properties of FeSe and its close cousins. This family of materials has attracted considerable attention due to the discovery of unexpected superconducting gap structures, a wide range of superconducting critical temperatures, and evidence for nontrivial band topology, including associated spin-helical surface states and vortex-induced Majorana bound states. Here, we review superconductivity in iron chalcogenide superconductors, including bulk FeSe, doped bulk FeSe, FeTe1−xSex, intercalated FeSe materials, and monolayer FeSe and FeTe1−xSex on SrTiO3. We focus on the superconducting properties, including a survey of the relevant experimental studies, and a discussion of the different proposed theoretical pairing scenarios. In the last part of the paper, we review the growing recent evidence for nontrivial topological effects in FeSe-related materials, focusing again on interesting implications for superconductivity.

Magnetism and superconductivity in Fe1+y Te1−xSex

Neutron scattering has played a significant role in characterizing magnetic and structural correlations in Fe1+y Te1−xSex and their connections with superconductivity. Here we review several key aspects of the physics of iron chalcogenide superconductors where neutron studies played a key role. These topics include the phase diagram of Fe1+y Te1−xSex, where the doping-dependence of structural transitions can be understood from a mapping to the anisotropic random field Ising model. We then discuss orbital-selective Mott physics in the Fe chalcogenide series, where temperature-dependent magnetism in the parent material provided one of the earliest cases for orbital-selective correlation effects in a Hund’s metal. Finally, we elaborate on the character of local magnetic correlations revealed by neutron scattering, its dependence on temperature and composition, and the connections to nematicity and superconductivity.

Importance of the Fermi surface and magnetic interactions for the superconducting dome in electron-doped FeSe intercalates

The van-der-Waals gap of iron chalcogenide superconductors can be intercalated with a variety of inorganic and organic compounds that modify the electron doping level of the iron layers. In Lix(C3N2H10)0.37FeSe, a dome in the superconducting transition temperature Tc has been reported to occur in the doping range of x=0.06 to x=0.68. We use a combination of density functional theory and spin fluctuation theory to capture the evolution of superconducting transition temperatures theoretically. We clearly demonstrate how the changing electronic structure supports an increasing superconducting Tc. The suppression of Tc at high doping levels can, however, only be understood by analyzing the magnetic tendencies, which evolve from stripe-type at low doping to bicollinear at high doping.