Fe-pnictide Superconductors Research Articles

Hydrothermal synthesis of tetragonal FeS: Dome-shaped superconductivity vs Fe:S actual molar ratios

We successfully synthesized tetragonal FeS with various Fe:S molar ratios using a hydrothermal method, and the EDS and XRF results confirmed that FeS exhibits superconductivity within the Fe and S element ratio range of 1.155–1.274, rather than a strict stoichiometric ratio. The reaction temperature can not only play a crucial role in determining the purity of the obtained FeS phase but also significantly alter its micromorphology. Significantly, by analyzing the relationship between the Fe:S actual molar ratio and Tc as well as the Fe:S actual molar ratio and unit cell volume, FeS exhibits dome-shaped superconductivity and shows a negative correlation with Tc and chemical pressure. Furthermore, considering the correlation between anion height (hanion) and Tc, Tc reaches the maximum value of 4.53 K for hanion ≈ 1.28 Å, a behavior distinct from that of observed in Fe-pnictide superconductors. In short, our experimental results provide a unique perspective to deepen our understanding of FeS superconductors.

Doping-dependent superconducting physical quantities of K-doped BaFe_2As_2 obtained through infrared spectroscopy

We investigated four single crystals of K-doped BaFe_2As_2 (Ba-122), Ba_{1-x}K_xFe_2As_2 with x = 0.29, 0.36, 0.40, and 0.51, using infrared spectroscopy. We explored a wide variety of doping levels, from under- to overdoped. We obtained the superfluid plasma frequencies (Omega _{textrm{sp}}) and corresponding London penetration depths (uplambda _{textrm{L}}) from the measured optical conductivity spectra. We also extracted the electron-boson spectral density (EBSD) functions using a two-parallel charge transport channel approach in the superconducting (SC) state. From the extracted EBSD functions, the maximum SC transition temperatures (T_c^{textrm{Max}}) were determined using a generalized McMillan formula and the SC coherence lengths (xi _{textrm{SC}}) were calculated using the timescales encoded in the EBSD functions and reported Fermi velocities. We identified some similarities and differences in the doping-dependent SC quantities between the K-doped Ba-122 and the hole-doped cuprates. We expect that the various SC quantities obtained across the wide doping range will provide helpful information for establishing the microscopic pairing mechanism in Fe-pnictide superconductors.

Multiplicity, Parity and Angular Momentum of a Cooper Pair in Unconventional Superconductors of D4h Symmetry: Sr2RuO4 and Fe-Pnictide Materials

Sr2RuO4 and Fe-pnictide superconductors belong to the same point group symmetry D4h. Many experimental data confirm odd pairs in Sr2RuO4 and even pairs in Fe-pnictides, but opposite conclusions also exist. Recent NMR results of Pustogow et al., which revealed even Cooper pairs in Sr2RuO4, require reconsideration of symmetry treatment of its SOP (superconducting order parameter). In the present work making use of the Mackey–Bradley theorem on symmetrized squares, a group theoretical investigation of possible pairing states in D4h symmetry is performed. It is obtained for I4/mmm , i.e., space group of Sr2RuO4, that triplet pairs with even spatial parts are possible in kz direction and in points M and Y. For the two latter cases pairing of equivalent electrons with nonzero total momentum is proposed. In P4/nmm space group of Fe- pnictides in point M, even and odd pairs are possible for singlet and triplet cases. It it shown that even and odd chiral states with angular momentum projection m=±1 have nodes in vertical planes, but Eg is nodal , whereas Eu is nodeless in the basal plane. It is also shown that the widely accepted assertion that the parity of angular momentum value is directly connected with the spatial parity of a pair is not valid in a space-group approach to the wavefunction of a Cooper pair.

Strain-Stabilized (π, π) Order at the Surface of Fe1+xTe.

A key property of many quantum materials is that their ground state depends sensitively on small changes of an external tuning parameter, e.g., doping, magnetic field, or pressure, creating opportunities for potential technological applications. Here, we explore tuning of the ground state of the nonsuperconducting parent compound, Fe1+xTe, of the iron chalcogenides by uniaxial strain. Iron telluride exhibits a peculiar (π, 0) antiferromagnetic order unlike the (π, π) order observed in the Fe-pnictide superconductors. The (π, 0) order is accompanied by a significant monoclinic distortion. We explore tuning of the ground state by uniaxial strain combined with low-temperature scanning tunneling microscopy. We demonstrate that, indeed under strain, the surface of Fe1.1Te undergoes a transition to a (π, π)-charge-ordered state. Comparison with transport experiments on uniaxially strained samples shows that this is a surface phase, demonstrating the opportunities afforded by 2D correlated phases stabilized near surfaces and interfaces.

Multigap Superconductivity in RbCa2Fe4As4F2 Investigated Using μSR Measurements

The superconducting properties of the recently discovered double Fe$_2$As$_2$ layered high-$T_c$ superconductor RbCa$_2$Fe$_4$As$_4$F$_2$ with $T_c\approx$ 30~K have been investigated using magnetization, heat capacity, transverse-field (TF) and zero-field (ZF) muon-spin rotation/relaxation ($\mu$SR) measurements. Our low field magnetization measurements and heat capacity (C$_p$) reveal an onset of bulk superconductivity with $T_{\bf c}\sim$ 30.0(4) K. Furthermore, the heat capacity exhibits a jump at $T_{\bf c}$ of $\Delta$C$_p$/$T_{\bf c}$=94.6 (mJ/mole-K$^2$) and no clear effect of applied magnetic fields was observed on C$_p$(T) up to 9 T between 2 K and 5 K. Our analysis of the TF-$\mu$SR results shows that the temperature dependence of the magnetic penetration depth is better described by a two-gap model, either isotropic $s$+$s$-wave or $s$+$d$-wave than a single gap isotropic $s$-wave or $d$-wave model for the superconducting gap. The presence of two superconducting gaps in RbCa$_2$Fe$_4$As$_4$F$_2$ suggests a multiband nature of the superconductivity, which is consistent with the multigap superconductivity observed in other Fe-based superconductors, including ACa$_2$Fe$_4$As$_4$F$_2$ (A=K and Cs). Furthermore, from our TF-$\mu$SR study we have estimated an in-plane penetration depth $\lambda_{\mathrm{ab}}$$(0)$ =231.5(3) nm, superconducting carrier density $n_s = 7.45 \times 10^{26}~ $m$^{-3}$, and carrier's effective-mass $m^*$ = 2.45\textit{m}$_{e}$. Our ZF $\mu$SR measurements do not reveal a clear sign of time reversal symmetry breaking at $T_{\bf c}$, but the temperature dependent relaxation between 150 K and 1.2 K might indicate the presence of spin-fluctuations. The results of our present study have been compared with those reported for other Fe pnictide superconductors.

Structural phase transition, precursory electronic anomaly, and strong-coupling superconductivity in quasi-skutterudite (Sr1−xCax)3Ir4Sn13 and Ca3Rh4Sn13**Project supported by the National Natural Science Foundation of China (Grant Nos. 11674377 and 11634015), the National Key R&D Program of China (Grant Nos. 2017YFA0302904 and 2016YFA0300502), and the Strategic Priority Research Program (B) of the Chinese Academy of Sciences (Grant No. XDB07020200). J. Y. is supported

The interplay between superconductivity and structural phase transition has attracted enormous interest in recent years. For example, in Fe-pnictide high temperature superconductors, quantum fluctuations in association with structural phase transition have been proposed to lead to many novel physical properties and even the superconductivity itself. Here we report a finding that the quasi-skutterudite superconductors (Sr1−xCax)3Ir4Sn13 (x = 0, 0.5, 1) and Ca3Rh4Sn13 show some unusual properties similar to the Fe-pnictides, through 119Sn nuclear magnetic resonance (NMR) measurements. In (Sr1−xCax)3Ir4Sn13, the NMR linewidth increases below a temperature T* that is higher than the structural phase transition temperature Ts. The spin-lattice relaxation rate (1/T1) divided by temperature (T), 1/T1T and the Knight shift K increase with decreasing T down to T*, but start to decrease below T*, and followed by more distinct changes at Ts. In contrast, none of the anomalies is observed in Ca3Rh4Sn13 that does not undergo a structural phase transition. The precursory phenomenon above the structural phase transition resembles that occurring in Fe-pnictides. In the superconducting state of Ca3Ir4Sn13, 1/T1 decays as exp(−Δ/kBT) with a large gap Δ = 2.21kBTc, yet without a Hebel–Slichter coherence peak, which indicates strong-coupling superconductivity. Our results provide new insight into the relationship between superconductivity and the electronic-structure change associated with structural phase transition.

Hidden phase in parent Fe-pnictide superconductors

We investigate the origin of exoticity in Fe-based systems via studying the Fermiology of CaFe2As2 employing Angle Resolved Photoemission spectroscopy (ARPES). While the Fermi surfaces (FSs) at 200 K and 31 K are observed to exhibit two dimensional (2D) and three dimensional (3D) topology, respectively, the FSs at intermediate temperatures reveal emergence of the 3D topology at much lower temperature than the structural & magnetic phase transition temperature (170 K, for the sample under scrutiny). This leads to the conclusion that the evolution of FS topology is not directly driven by the structural transition. In addition, we discover the existence in ambient conditions of energy bands related to the collapsed tetragonal (cT) phase. These bands are distinctly resolved in the high-photon energy spectra exhibiting strong Fe 3d character. They gradually move to higher binding energies due to thermal compression with cooling, leading to the emergence of 3D topology in the Fermi surface. These results reveal the so-far hidden existence of a cT phase in ambient conditions, which is argued to lead to quantum fluctuations responsible for the exotic electronic properties in Fe-pnictide superconductors.

A density functional theory study of the influence of exchange-correlation functionals on the properties of FeAs

We use density functional theory within the local density approximation (LDA), LDA + U, generalised gradient approximation (GGA), GGA + U, and hybrid-functional methods to calculate the properties of iron monoarsenide. FeAs, which forms in the MnP structure, is of current interest for potential spintronic applications as well as being the parent compound for the pnictide superconductors. We compare the calculated structural, magnetic and electronic properties obtained using the different functionals to each other and to experiment, and investigate the origin of a recently reported magnetic spiral. Our results indicate the appropriateness or otherwise of the various functionals for describing FeAs and the related Fe-pnictide superconductors.

Phase stability and large in-plane resistivity anisotropy in the 112-type iron-based superconductor Ca1−xLaxFeAs2

The recently discovered high-T$_c$ superconductor Ca$_{1-x}$La$_{x}$FeAs$_{2}$ is a unique compound not only because of its low symmetry crystal structure, but also because of its electronic structure which hosts Dirac-like metallic bands resulting from (spacer) zig-zag As chains. We present a comprehensive first principles theoretical study of the electronic and crystal structures of Ca$_{1-x}$La$_{x}$FeAs$_{2}$. After discussing the connection between the crystal structure of the 112 family, which Ca$_{1-x}$La$_{x}$FeAs$_{2}$ is a member of, with the other known structures of Fe pnictide superconductors, we check the thermodynamic phase stability of CaFeAs$_{2}$, and similar hyphothetical compounds SrFeAs$_{2}$ and BaFeAs$_{2}$ which, we find, are slightly higher in energy. We calculate the optical conductivity of Ca$_{1-x}$La$_{x}$FeAs$_{2}$ using the DFT + DMFT method, and predict a large in-plane resistivity anisotropy in the normal phase, which does not originate from electronic nematicity, but is enhanced by the electronic correlations. In particular, we predict a 0.34 eV peak in the $yy$ component of the optical conductivity of the 30\% La doped compound, which correponds to coherent interband transitions within a fast-dispersing band arising from the zig-zag As-chains which are unique to this compound. We also study the Landau free energy for Ca$_{1-x}$La$_{x}$FeAs$_{2}$ including the order parameter relevant for the nematic transition and find that the free energy does not have any extra terms that could induce ferro-orbital order. This explains why the presence of As chains does not broaden the nematic transition in Ca$_{1-x}$La$_{x}$FeAs$_{2}$.

Self-hole-doping–induced superconductivity in KCa2Fe4As4F2

The electronic structure, magnetism, Fermi surface nesting, and bare susceptibility of the superconductor KCa2Fe4As4F2 are discussed in relation to the Fe-pnictide superconductors based on the first-principle calculations. There are ten bands crossing the Fermi level in the nonmagnetic (NM) states, resulting in six hole-like Fermi surface (FS) sheets along the line and four electron-like FS sheets along the line. It is more complicated than other FeAs-based superconductors, showing multi-bands character. Fixed spin moment calculations and the total energies of different magnetic phase indicate that KCa2Fe4As4F2 has a strong tendency towards magnetism, i.e., the stripe antiferromagnetic state. But the self-hole-doping suppressed the spin-density wave state, and then induced superconductivity in the parent compound. Such self-doping strategy may be used for future exploration of new superconductors.

ThFeAsN in relation to other iron-based superconductors

The electronic structure, magnetic and structural properties of the superconductor ThFeAsN are discussed in relation to the Fe-pnictide and Fe-chalcogenide superconductors based on results of first principles calculations. The electronic structure is that of a high density of states semimetal. It shows approximately nested hole and electron Fermi surfaces of Fe d character involving the xz, yz and xy orbitals. There is a strong tendency towards magnetism at the GGA level, and this magnetism is important for describing the FeAs bonding, but greatly overestimates the magnetic ordering. The lowest energy magnetic state at the GGA level is the stripe order, and this particular order couples strongly to electrons near EF. ThFeAsN is therefore strongly similar to the Fe-pnictide family of superconductors, although it is a particularly anisotropic member.

Multiple Antiferromagnetic Spin Fluctuations and Novel Evolution of Tc in Iron-Based Superconductors LaFe(As1−xPx)(O1−yFy) Revealed by 31P-NMR Studies

We report on 31P-NMR studies of LaFe(As_{1-x}P_x)(O_{1-y}F_{y}) over wide compositions for 0<x<1 and 0<y<0.14, which provide clear evidence that antiferromagnetic spin fluctuations (AFMSFs) are one of the indispensable elements for enhancing Tc. Systematic 31P-NMR measurements revealed two types of AFMSFs in the temperature evolution, that is, one is the AFMSFs that develop rapidly down to Tc with low-energy characteristics, and the other, with relatively higher energy than the former, develops gradually upon cooling from high temperature. The low-energy AFMSFs in low y (electron doping) over a wide x (pnictogen height suppression) range are associated with the two orbitals of d_{xz/yz}, whereas the higher-energy ones for a wide y region around low x originate from the three orbitals of d_{xy} and d_{xz/yz}. We remark that the nonmonotonic variation of Tc as a function of x and y in LaFe(As_{1-x}P_x)(O_{1-y}F_y) is attributed to these multiple AFMSFs originating from degenerated multiple 3d orbitals inherent to Fe-pnictide superconductors.

Electronic structures and magnetism of LaFe2Ge2 and LaFe2Si2: First-principles studies

Inspired by the recent discovery of superconductivity in YFe2Ge2, we report first-principles calculations on the electronic structure and magnetic properties of LaFe2Ge2 and LaFe2Si2. We found that LaFe2Ge2 and LaFe2Si2 share similar electronic structure and magnetism properties. In the nonmagnetic state, the density of states at the Fermi level are mostly derived from the dxy, dyz, and dzx orbits, just like the Fe-pnictide superconductors. The band structure and Fermi surfaces exhibit significantly three dimensional character. Our calculations indicate that the ground state of LaFe2Ge2 and LaFe2Si2 is the stripe antiferromagnetic configuration in the a-b plane and stacked antiparallel along the c-axis direction. The overestimate magnetic tendency within calculation indicates these systems nearness to a magnetic quantum critical point (QCP).

Structural and magnetic phase transitions inCa0.73Le0.27FeAs2with electron-overdoped FeAs layers

We report a study of the Ca$_{0.73}$La$_{0.27}$FeAs$_2$ single crystals. We unravel a monoclinic to triclinic phase transition at 58 K, and a paramagnetic to stripe antiferromagnetic (AFM) phase transition at 54 K, below which spins order 45$^\circ$ away from the stripe direction. Furthermore, we demonstrate this material is substantially structurally untwinned at ambient pressure with the formation of spin rotation walls (S-walls). Finally, in addition to the central-hole and corner-electron Fermi pockets usually appearing in Fe pnictide superconductors, angle-resolved photoemission (ARPES) measurements resolve a Fermiology where an extra electron pocket of mainly As chain character exists at the Brillouin zone edge.

Specific Heat of Ba0.59K0.41Fe2As2, an Fe-Pnictide Superconductor with Tc = 36.9 K, and a New Method for Identifying the Electron Contribution

We report measurements of the specific heat of Ba$_{0.59}$K$_{0.41}$Fe$_{2}$As$_{2}$, an Fe-pnictide superconductor with $T_c$ = 36.9 K, for which there are suggestions of an unusual electron pairing mechanism. We use a new method of analysis of the data to derive the parameters characteristic of the electron contribution. It is based on comparisons of ${\alpha}$-model expressions for the electron contribution with the total measured specific heat, which give the electron contribution directly. It obviates the need in the conventional analyses for an independent, necessarily approximate, determination of the lattice contribution, which is subtracted from the total specific heat to obtain the electron contribution. It eliminates the uncertainties and errors in the electron contribution that follow from the approximations in the determination of the lattice contribution. Our values of the parameters characteristic of the electron contribution differ significantly from those obtained in conventional analyses of specific-heat data for five similar hole-doped BaFe$_{2}$As$_{2}$ superconductors, which also differ significantly among themselves. They show that the electron density of states is comprised of contributions from two electron bands with superconducting-state energy gaps that differ by a factor 3.8, with 77$\%$ coming from the band with the larger gap. The variation of the specific heat with magnetic field is consistent with extended $s$-wave pairing, one of the theoretical predictions. The relation between the densities of states and the energy gaps in the two bands is not consistent with a theoretical model based on interband interactions alone. Comparison of the normal-state density of states with band-structure calculations shows an extraordinarily large effective mass enhancement, for which there is no precedent in similar materials and no theoretical explanation.

Electronic Properties of BaFe2As2 upon Doping and Pressure: The Prominent Role of the As p Orbitals.

Using high-resolution, lifetime removed, x-ray absorption spectroscopy at the As K edge, we evidence the strong sensitivity of the As electronic structure upon electron doping with Co or pressure change in BaFe2As2, at room temperature. Our results unravel the prominent role played by As-4p orbitals in the electronic properties of the Fe pnictide superconductors. We propose a unique picture to describe the overall effect of both external parameter doping and pressure, resolving the apparent contradiction between angle-resolved photoemission spectroscopy, transport, and absorption results, with the As-p states as a key ingredient.

Spectroscopic evidence for strong quantum spin fluctuations with itinerant character inYFe2Ge2

We report x-ray absorption and photoemission spectroscopy of the electronic structure in the normal state of metallic YFe2Ge2. The data reveal evidence for large fluctuating spin moments on the Fe sites, as indicated by exchange multiplets appearing in the Fe 3s core level photoemission spectra, even though the compound does not show magnetic order. The magnitude of the multiplet splitting is comparable to that observed in the normal state of the Fe-pnictide superconductors. This shows a connection between YFe2Ge2 and the Fe-based superconductors even though it contains neither pnictogens nor chalcogens. The implication is that the chemical range of compounds showing at least one of the characteristic magnetic signatures of the Fe-based superconductors is broader than previously thought.

Emergence of Novel Antiferromagnetic Order Intervening between Two Superconducting Phases in LaFe(As1−xPx)O: 31P-NMR Studies

We revealed novel phase deagram of Fe-pnictide high-Tc superconductor LaFe(As_{1-x}P_{x})O in wide doping level (0.3<x<1) by P-NMR. Systematic 31P-NMR studies revealed the emergence of the antiferromagnetic ordered phase (AFM-2) in 0.4 < x < 0.7 that intervenes between two superconductivity (SC-1/SC-2) phases. The 31P-NMR Knight shift points to the appearance of the sharp density of states at the Fermi level that is derived from d_{3Z^2?r^2} orbit, which is less relevant with the onset of the SC-2. On the other hand, we remark that the AFM spin fluctuations arising from the interband nesting on the d_{XZ}/d_{YZ} orbits must be a key ingredient for the occurrence of SC around AFM-2.

Small and nearly isotropic hole-like Fermi surfaces in LiFeAs detected through de Haas–van Alphen effect

LiFeAs is unique among the arsenic based Fe-pnictide superconductors because it is the only nearly stoichiometric compound which does not exhibit magnetic order. This is at odds with electronic structure calculations which find a very stable magnetic state and predict cylindrical hole- and electron-like Fermi surface sheets whose geometry suggests spin fluctuations and a possible instability toward long-range ordering at the nesting vector. In fact, a complex magnetic phase diagram is indeed observed in the isostructural NaFeAs compound. Previous angle-resolved photoemission (ARPES) experiments revealed the existence of both hole and electron-like surfaces, but with rather distinct cross-sectional areas and an absence of the nesting that is thought to underpin both magnetic order and superconductivity in the pnictide family of superconductors. These ARPES observations were challenged by subsequent de Haas--van Alphen (dHvA) measurements which detected a few, electron-like Fermi surface sheets in rough agreement with the original band calculations. Here, we show a detailed dHvA study unveiling additional, small and nearly isotropic Fermi surface sheets in LiFeAs single crystals, which ought to correspond to hole-like orbits, as previously observed by ARPES. Therefore, our results reconcile the apparent discrepancy between ARPES and the previous dHvA results. The small size of these Fermi surface pockets suggests a prominent role for the electronic correlations in LiFeAs. The absence of gap nodes, in combination with the coexistence of quasi-two-dimensional and three-dimensional Fermi surfaces, favor an $s$-wave pairing symmetry for LiFeAs. But similar electron-like Fermi surfaces combined with very different hole pockets between LiFeAs and LiFeP suggest that the nodes in the gap function of LiFeP might be located on the hole pockets. This would be difficult to reconcile with the current understanding of the $s\ifmmode\pm\else\textpm\fi{}$ scenario.

Possible s±-wave pairing evidenced by midgap surface bound states in Fe-pnictide superconductors

A phenomenological theory of tunneling spectroscopy for Fe-pnictide superconductors is developed by taking into consideration asymmetric interface scattering between particle and holes. It is shown that, consistent with anti-phase s±-wave pairing, appreciable zero-energy surface bound states exist on the [100] surface of Fe-pnictide superconductors. However, in contrast to the [110] bound states in d-wave cuprate superconductors, these bound states arise as a result of non-conservation of momentum perpendicular to the interface for tunneling electrons and the s± pairing, and hence they can only exist in a small window (∼ ± 6∘) in the orientation of edges near the [100] direction. Our results explain why a zero-bias conductance peak is often observed in tunneling spectroscopy and why, when it disappears, two coherent peaks show up. These results provide unambiguous signals to test for possible s±-wave pairing in Fe-pnictide superconductors.