Fe-based Superconductors Research Articles

Observation of anion-stoichiometry phase separation in Fe(Te,Se) film

Nanostructure control is of fundamental and technological importance because various properties such as vortex pinning in superconductors are determined by the nanostructure. While the nanostructure in superconducting oxides is well controlled, the nanostructure control of iron-based superconductors is required. The nanostructure has not yet been well controlled even in Fe(Te,Se) with the simplest structure among Fe-based superconductors because the anion may be non-stoichiometric and anionic substitution is possible. In this study, we observed the compositional inhomogeneity originating from phase separation in Fe(Te,Se) films, which were prepared by pulsed laser deposition. The films deposited at lower temperature do not show nanoscale compositional inhomogeneity. On the other hand, the high-temperature deposited films contain an inhomogeneous anion distribution with the size of ∼8 nm due to phase separation. The spacing of the compositional inhomogeneity is ∼16 nm. This structure obtained by phase separation is expected to be an effective pinning center in high magnetic fields after further optimization. Thus, the method of nanostructure control other than nanocomposite formation in oxides is demonstrated for Fe(Te,Se).

Pressure-induced antiferromagnetic-tetragonal to nonmagnetic-collapse-tetragonal insulator-metal transition in ThMnAsN

We report first-principles numerical discovery of hydrostatic pressure-driven tetragonal to collapsed tetragonal transition in 1111-type material ThMnAsN accompanied by simultaneous magneto-structural, insulator to metal transition together with complete collapse of Mn moments. We present detailed evolution of various structural parameters, magnetism and electronic structures of ThMnAsN with increasing hydrostatic pressure. All the structural parameters show anomalies at a critical pressure $$P_\text {c} \sim$$ 8.1 GPa; c-lattice parameter, out-of-plane As–As bond length, anion height ( $$h_\text {As}$$ ) undergo drastic modifications compared to the in-plane parameters which is manifested in an iso-structural phase transition from tetragonal to a collapsed tetragonal (cT) phase. These modifications in “local structural correlations” due to pressure destroy the usually localized nature of Mn moments which gets completely quenched. Apart from that the elastic constant, the electronic structures also bear the finger prints of insulator-metal and magneto-structural transition at higher pressures accompanying a total collapse of magnetic moment at the vicinity of $$P_\text {c}$$ . The critical value of the pressure $$P_\text {c}$$ at which tetragonal to collapse tetragonal phase transition occurs, remains robust with respect to the on-site Hubbard correlation (U). The dynamical stability of the compound at higher pressures (above and below the magneto-structural transition) is affirmed through detailed computations of phonon dispersion curves endowed with positive phonon frequency throughout the Brillouin zone. The effect of magnetic spin structure on the electronic band structures is obtained through band unfolding. The electronic structure of ThMnAsN at higher pressures “orbital selectively” influences bands, band gap and closely resembles with the electronic structure of Fe-based superconductors (quasi-two-dimensional Fermi surfaces) with the occurrences of orbital-selective Lifshitz transition.

Magnetotransport property of oxygen-annealed Fe1+y Te thin films

Fe-based superconductors are one of the current research focuses. FeTe is unique in the series of FeSe1−x Te x , since it is nonsuperconducting near the FeTe side in the phase diagram in contrast to the presence of superconductivity in other region. However, FeTe thin films become superconducting after oxygen annealing and the mechanism remains elusive. Here, we report the temperature dependences of resistivity, Hall effect and magnetoresistance (MR) of a series of FeTe thin films with different amounts of excess Fe and oxygen. These properties show dramatic changes with excess Fe and oxygen incorporation. We found the Hall coefficients are positive for the oxygen-annealed samples, in contrast to the transition from positive to negative below 50 K for the vacuum-annealed samples. For all samples, both the resistivity and Hall coefficient show a dramatic drop, respectively, at around 50 K–75 K, implying coexistence of superconductivity and antiferromagnetic order for the oxygen-annealed samples. The vacuum-annealed samples show both positive and negative values of MR depending on temperature, while negative MR dominates for the oxygen-annealed samples. We also found that oxygen annealing reduces the excess Fe in FeTe, which has been neglected before. The results are discussed in terms of several contributions, and a comparison is made between the oxygen-annealed FeTe thin films and FeSe1−x Te x . This work is helpful for shedding light on the understanding of oxygen-annealed FeTe thin films.

A Study of the Temperature-Dependent Surface and Upper Critical Magnetic Fields in KFeSe and LaSrCuO Superconductors

The critical magnetic field is one of the most interesting properties of superconductors. Thus, this study aimed to investigate the surface and upper critical magnetic fields of superconductors in Fe-based and cuprate superconductors as KFeSe and LaSrCuO superconductors, respectively. The anisotropic two-band Ginzburg–Landau method was used to generate the analytic equation. The analytics were shown for the simplified equation so that a second-order polynomial temperature-dependent equation could be applied and fitted to the experimental results of KFeSe and LaSrCuO superconductors. After that, numerical calculations were applied to find the shape of the Fermi surface, which is an important component within the band structure. It was found that the anisotropy of the Fermi surface for each band structure was affected by the upper critical magnetic field and the surface critical magnetic field to the upper critical magnetic field of the superconductors. The second-order polynomial temperature-dependent model can be applied to other superconductors to predict the surface and upper critical magnetic fields.

Symmetry of Identical Particles, Modern Achievements in the Pauli Exclusion Principle, in Superconductivity and in Some Other Phenomena

In this review, the modern achievements in studies of the Pauli exclusion principle (PEP) and the properties of the identical particle systems when PEP is not fulfilled are discussed. The validity of conception of the spin in the framework of density functional theory (DFT) approaches is analyzed. The modern state of the recently discovered Fe-based superconductors is discussed in detail. These materials belong to the paramagnetic semimetal family and become superconductors upon doping. Recently, in 2020, room-temperature superconductivity was realized. However, from the following discussion in the SC community, it was not evident that the results of room-temperature superconductivity have been repeated by other laboratories. Thus, the question “is room temperature really achieved?” is still open. In the concluding remarks, we present the explanation of why the PEP limitations on the symmetry of identical particles system exist in nature, and following from it, some important consequences.

Colossal negative magnetoresistance in spin glass Na(Zn,Mn)Sb

We report the study of magnetic and transport properties of polycrystalline and single crystal Na(Zn,Mn)Sb, a new member of “111” type of diluted magnetic materials. The material crystallizes into Cu2Sb-type structure which is isostructural to “111” type Fe-based superconductors. With suitable carrier and spin doping, the Na(Zn,Mn)Sb establishes spin-glass ordering with freezing temperature (T f ) below 15 K. Despite lack of long-range ferromagnetic ordering, Na(Zn,Mn)Sb single crystal still shows sizeable anomalous Hall effect below T f . Carrier concentration determined by Hall effect measurements is over 1019 cm–3. More significantly, we observe colossal negative magnetoresistance (MR ≡ [ρ(H) − ρ(0)]/ρ(0)) of –94% in the single crystal sample.

Inhomogeneous Superconductivity Onset in FeSe Studied by Transport Properties

Heterogeneous superconductivity onset is a common phenomenon in high-Tc superconductors of both the cuprate and iron-based families. It is manifested by a fairly wide transition from the metallic to zero-resistance states. Usually, in these strongly anisotropic materials, superconductivity (SC) first appears as isolated domains. This leads to anisotropic excess conductivity above Tc, and the transport measurements provide valuable information about the SC domain structure deep within the sample. In bulk samples, this anisotropic SC onset gives an approximate average shape of SC grains, while in thin samples, it also indicates the average size of SC grains. In this work, both interlayer and intralayer resistivity were measured as a function of temperature in FeSe samples of various thicknesses. To measure the interlayer resistivity, FeSe mesa structures oriented across the layers were fabricated using FIB. As the sample thickness decreases, a significant increase in superconducting transition temperature Tc is observed: Tc raises from 8 K in bulk material to 12 K in microbridges of thickness ∼40 nm. We applied analytical and numerical calculations to analyze these and earlier data and find the aspect ratio and size of the SC domains in FeSe consistent with our resistivity and diamagnetic response measurements. We propose a simple and fairly accurate method for estimating the aspect ratio of SC domains from Tc anisotropy in samples of various small thicknesses. The relationship between nematic and superconducting domains in FeSe is discussed. We also generalize the analytical formulas for conductivity in heterogeneous anisotropic superconductors to the case of elongated SC domains of two perpendicular orientations with equal volume fractions, corresponding to the nematic domain structure in various Fe-based superconductors.

Observations of Nematicity, Dopants, and Zero-Bias Conductance Peaks for the Ca0.9La0.1FeAs2 Superconductor

Ca1-xLaxFeAs2 (CLFA112) belongs to a new family of Fe-based superconductors (FeSCs) and has a unique crystal structure featuring an arsenic zigzag chain layer, which has been proposed to be a possible two-dimensional topological insulator. This suggests that CLFA112 is a potential topological superconductor-a platform to realize Majorana fermions. Up to now, even a clear superconducting (SC) gap in CLFA112 has never been observed, and the SC properties of CLFA112 remain largely elusive. In this letter, we report the results of an atomic-scale investigation of the electronic structure of CLFA112 crystals using low-temperature scanning tunneling microscopy (STM). We revealed four different types of surfaces exhibiting distinct electronic properties, with all surfaces displaying dominating 2 × 1 surface reconstructions. On a Ca/La layer on top of an FeAs layer, a clear SC gap of ~12 mV was observed only at the crevices (vacancies) where the FeAs layer can be directly accessed. Remarkably, the FeAs termination layer displayed a dispersing nematic modulation both in real and q space. We also present peculiar zero-bias conductance peaks for the very As chain layer that is believed to exhibit a topological edge state as well as the influence of La dopants on the As chain layer.

Rigorous formalism for unconventional symmetry breaking in Fermi liquid theory and its application to nematicity in FeSe

Unconventional symmetry breaking due to nonlocal order parameters has attracted considerable attention in many strongly correlated metals. Famous examples are the nematic order in Fe-based superconductors and the star-of-David charge density order in kagome metals. Such exotic symmetry breaking in metals is a central issue of modern condensed matter physics, while its theoretical foundation is still unclear in comparison with the well-established theory of superconductivity. To overcome this difficulty, here we introduce the "form factor" that generalizes the nonlocal order parameter into the Luttinger-Ward (LW) Fermi liquid theory. We then construct a rigorous formalism of the "density-wave equation" that gives the thermodynamically stable form factor, similarly to the superconducting-gap equation. In addition, a rigorous expression of the Ginzburg-Landau free-energy for the unconventional order is presented to calculate various thermodynamic properties. In the next stage, we apply the derived formalism to a typical Fe-based superconductor FeSe, by using the one-loop LW function that represents the free-energy gain due to the interference among paramagnons. The following key experiments are naturally explained: (i) Lifshitz transition (=disappearance of an electron-pocket) due to the bond+orbital order below $T_c$. (ii) Curie-Weiss behavior of the nematic susceptibility at higher T, and the deviation from the Curie-Weiss behavior at lower T near the nematic quantum-critical-point. (iii) Scaling relation of the specific heat jump at $T_c$, $\Delta C/T_c \propto T_c^b$ with $b \sim 3$. (Note that b=0 in the BCS theory.) These results lead to a conclusion that the nematicity in FeSe is the bond+orbital order due to the "paramagnon interference mechanism". The present theory paves the way for solving various unconventional phase transition systems.

Rotation of the dislocation grid in multilayer FeSe films and visualization of electronic nematic domains via orbital-selective tunneling

Understanding the interplay of structural and electronic symmetry breaking in Fe-based high temperature superconductors remains of high interest. In this work we grow strain-patterned multilayer FeSe thin films in a range of thicknesses using molecular beam epitaxy. We study the formation of electronic nematic domains and spatially-varying strain using scanning tunneling microscopy and spectroscopy. We directly visualize the formation of edge dislocations that give rise to a two-dimensional edge dislocation network in the films. Interestingly, we observe a 45 degree in-plane rotation of the dislocation network as a function of film thickness, yielding antisymmetric strain along different directions. This results in different coupling ratios between electronic nematic domains and antisymmetric strain. Lastly, we are able to distinguish between different orthogonal nematic domains by revealing a small energy-dependent difference in differential conductance maps between the two regions. This could be explained by orbital-selective tip-sample tunneling. Our observations bring new insights into the dislocation network formation in epitaxial thin films and provide another nanoscale tool to explore electronic nematicity in Fe-based superconductors.

Evidence for a robust sign-changing s-wave order parameter in monolayer films of superconducting Fe (Se,Te)/Bi2Te3

The Fe-based superconductor Fe (Se,Te) combines non-trivial topology with unconventional superconductivity and may be an ideal platform to realize exotic states such as high-order topological corner modes and Majorana modes. Thin films of Fe (Se,Te) are particularly important for device fabrication and phase sensitive transport measurements. While bulk Fe (Se,Te) has been extensively studied, the nature of the superconducting order parameter in the monolayer limit has not yet been explored. In this work, we study monolayer films of Fe (Se,Te) on Bi2Te3 with scanning tunneling spectroscopy. Monolayer Fe (Se,Te)/Bi2Te3 heterostructures host a multigap superconducting state that strongly resembles the bulk. Analysis of the phase-referenced quasiparticle interference signal reveals a sign-changing s-wave order parameter similar to the bulk as well as a unique pattern of sign changes which have not been observed in the bulk. Our work establishes monolayer Fe (Se,Te)/Bi2Te3 as a robust multi-band unconventional superconductor and sets the stage for explorations of non-trivial topology in this highly-tunable system.

Electronic structure, magnetic order and Lifshitz transition in electron doped new structure 12442 type Fe-based superconductors

We investigate in detail the electronic structure of very recently discovered electron doped 12442-type iron based BaTh2Fe4As4(N1−xOx)2 compounds (x = 0.1–0.6), using Density Functional Theory (DFT) based first principles calculations. Unlike in many iron-based superconducting compounds, absence of As-4pZ orbital character, and dominant contributions from Fe-3d orbitals close to the Fermi level are noted. Formation energy calculations indicate x = 0.3 structure is the most stable which is consistent with experimental observation. Incorporating magnetic order at Fe sites in compound x = 0.3, our calculations predict stripe AFM as ground state magnetic structure. Calculated Arsenic height from the Fe square plane (hAs) for striped AFM configuration agrees well with the experiment. An important outcome of this calculation is the prediction of occurrence of Lifshitz transition at the same doping level (x = 0.6) for which the highest critical temperature is reported in literature. Detailed analysis of electronic structure results like estimation of radii of various Fermi pockets, orbital characters of Fermi surfaces lead to prediction of mixed d and s pairing symmetry.

Thermodynamic approach for enhancing superconducting critical current performance

The addition of artificial pinning centers has led to an impressive increase in the critical current density (Jc) of superconductors, enabling record-breaking all-superconducting magnets and other applications. The Jc of superconductors has reached ~0.2–0.3 Jd, where Jd is the depairing current density, and the numerical factor depends on the pinning optimization. By modifying λ and/or ξ, the penetration depth and coherence length, respectively, we can increase Jd. For (Y0.77Gd0.23)Ba2Cu3Oy ((Y,Gd)123), we can achieve this by controlling the carrier density, which is related to λ and ξ. We can also tune λ and ξ by controlling the chemical pressure in Fe-based superconductors, i.e., BaFe2(As1−xPx)2 films. The variation in λ and ξ leads to an intrinsic improvement in Jc via Jd, allowing extremely high values of Jc of 130 MA/cm2 and 8.0 MA/cm2 at 4.2 K, consistent with an enhancement in Jd of a factor of 2 for both incoherent nanoparticle-doped (Y,Gd)123 coated conductors (CCs) and BaFe2(As1−xPx)2 films, showing that this new material design is useful for achieving high critical current densities in a wide array of superconductors. The remarkably high vortex-pinning force in combination with this thermodynamic and pinning optimization route for the (Y,Gd)123 CCs reached ~3.17 TN/m3 at 4.2 K and 18 T (H||c), the highest values ever reported for any superconductor.

Impact of atomic defects in the electronic states of FeSeS superconducting crystals

The electronic properties of Fe-based superconductors are drastically affected by deformations on their crystal structure introduced by doping and pressure. Here we study single crystals of FeSeS x and reveal that local crystal deformations such as atomic-scale defects impact the spectral shape of the electronic core level states of the material. By means of scanning tunneling microscopy we image S-doping induced defects as well as diluted dumbbell defects associated with Fe vacancies. We have access to the electronic structure of the samples by means of x-ray photoemission spectroscopy (XPS) and show that the spectral shape of the Se core levels can only be adequately described by considering a principal plus a minor component of the electronic states. We find this result for both pure and S-doped samples, irrespective that in the latter case the material presents extra crystal defects associated to doping with S atoms. We argue that the second component in our XPS spectra is associated with the ubiquitous dumbbell defects in FeSe that are known to entail a significant modification of the electronic clouds of surrounding atoms.

Hybridization of CaFe1−xCoxAsF (x = 0, 0.06, 0.11, 0.144) studied by x-ray absorption spectroscopy and ultraviolet photoemission spectroscopy

The parent compound CaFeAsF undergoes a structural phase transition from tetragonal to orthorhombic at T ∼ 121 K without superconductivity. The superconductivity emerged when the Fe sites are partially substituted by Co with a doping level of above 0.06 and the superconducting transition temperature is raised to 22 K in CaFe0.89Co0.11AsF. In this paper, the electronic structures of CaFe1−xCoxAsF (x = 0, 0.06, 0.11, 0.144) samples were studied by x-ray absorption spectroscopy (XAS). With the doping of Co, the Fe L3 XAS spectra shift to lower photon energy. Combined with the valence band spectra study, it is indicated that the strength of the hybridization between Fe 3d and As 4p is enhanced together with the increment of the superconducting transition temperature, after Co doping. The results suggest the enhancement of the hybridization between Fe 3d and As 4p plays an important role in the evolution of the superconductivity in Fe-based superconductors.

Superconductivity in the crystallogenide LaFeSiO1−δ with squeezed FeSi layers

Pnictogens and chalcogens are both viable anions for promoting Fe-based superconductivity, and intense research activity in the related families has established a systematic correlation between the Fe-anion height and the superconducting critical temperature Tc, with an optimum Fe-anion height of ~1.38 Å. Here, we report the discovery of superconductivity in the compound LaFeSiO1−δ that incorporates a crystallogen element, Si, and challenges the above picture: considering the strongly squeezed Fe–Si height of 0.94 Å, the superconducting transition at Tc = 10 K is unusually high. In the normal state, the resistivity displays non-Fermi-liquid behavior while NMR experiments evidence weak antiferromagnetic fluctuations. According to first-principles calculations, the Fermi surface of this material is dominated by hole pockets without nesting properties, which explains the strongly suppressed tendency toward magnetic order and suggests that the emergence of superconductivity materializes in a distinct set-up, as compared to the standard s±- and d-wave electron-pocket-based situations. These properties and its simple-to-implement synthesis make LaFeSiO1−δ a particularly promising platform to study the interplay between structure, electron correlations, and superconductivity.

Effect of S-doping on the magnetic and electrical properties of FeSe superconductor

Here we report on the magnetic and magneto-transport behavior of Fe-based superconductor with nominal compositions FeSe1−xSx (x=0.1 and 0.2). The impact of external hydrostatic pressure (P) and chemical pressure on the superconducting state of the FeSe system has been investigated in this work. Superconducting transition temperature (Tc) is found to be shifted towards higher temperatures with 10% S doping at the Se site of the FeSe alloy. On further increase in the doping concentration (for x=0.2), the superconducting Tc decreases. We have also observed a significant effect of external P on the superconducting properties of these S-doped alloys. Different superconducting parameters calculated from our experimental data confirm the type-II superconducting nature of the studied compounds. The signature of flux flow resistance is observed in the isothermal resistivity data as a function of the external magnetic field.

Stronger quantum fluctuation with larger spins: Emergent magnetism in the pressurized high-temperature superconductor FeSe

A counter-intuitive enhancement of quantum fluctuation with larger spins, together with a few novel physical phenomena, is discovered in studying the recently observed emergent magnetism in high-temperature superconductor FeSe under pressure. Starting with experimental crystalline structure from our high-pressure X-ray refinement, we analyze theoretically the stability of the magnetically ordered state with a realistic spin-fermion model. We find surprisingly that in comparison with the magnetically ordered Fe-pnictides, the larger spins in FeSe suffer even stronger long-range quantum fluctuation that diminishes their ordering at ambient pressure. This "fail-to-order" quantum spin liquid state then develops into an ordered state above 1GPa due to weakened fluctuation accompanying the reduction of anion height and carrier density. The ordering further benefits from the ferro-orbital order and shows the observed enhancement around 1GPa. We further clarify the controversial nature of magnetism and its interplay with nematicity in FeSe in the same unified picture for all Fe-based superconductors. In addition, the versatile itinerant carriers produce interesting correlated metal behavior in a large region of phase space. Our study establishes a generic exceptional paradigm of stronger quantum fluctuation with larger spins that complements the standard knowledge of insulating magnetism.

Quantum critical fluctuations in an Fe-based superconductor

Quantum critical fluctuations may prove to play an instrumental role in the formation of unconventional superconductivity. Here, we show that the characteristic scaling of a marginal Fermi liquid is present in inelastic light scattering data of an Fe-based superconductor tuned through a quantum critical point (QCP) by chemical substitution or doping. From the doping dependence of the imaginary time dynamics we are able to distinguish regions dominated by quantum critical behavior from those having classical critical responses. This dichotomy reveals a connection between the marginal Fermi liquid behavior and quantum criticality. In particular, the overlap between regions of high superconducting transition temperatures and quantum critical scaling suggests a contribution from quantum fluctuations to the formation of superconductivity.

Semi-classical simulation of spin-1 magnets

Theoretical studies of magnets have traditionally concentrated on either classical spins, or the extreme quantum limit of spin-1/2. However, magnets built of spin-1 moments are also intrinsically interesting, not least because they can support quadrupole, as well as dipole moments, on a single site. For this reason, spin-1 models have been extensively studied as prototypes for quadrupolar (spin-nematic) order in magnetic insulators, and Fe-based superconductors. At the same time, because of the presence of quadrupoles, the classical limit of a spin-1 moment is not an $O(3)$ vector, a fact which must be taken into account in describing their properties. In this Article we develop a method to simulate spin-1 magnets based on a $u(3)$ algebra which treats both dipole and quadrupole moments on equal footing. This approach is amenable to both classical and quantum calculations, and we develop the techniques needed to calculate thermodynamic properties through Monte Carlo simulations and classical low-temperature expansion, and dynamical properties, through "molecular dynamics" simulations and a multiple-boson expansion. As a case study, we present detailed analytic and numerical results for the thermodynamic properties of ferroquadrupolar order on the triangular lattice, and its associated dynamics. At low temperatures, we show that it is possible to "correct" for the effects of classical statistics in simulations, and extrapolate to the zero-temperature quantum results found in flavour-wave theory.