Iron Arsenide Superconductors Research Articles

Magnetoelastic coupling, negative thermal expansion, and two-dimensional magnetic excitations in FeAs

We present a temperature-dependent investigation of the local structure and magnetic dynamics of the FeAs binary. The magnetic susceptibility $\ensuremath{\chi}(T)$ result shows an anomalous broad feature up to 550 K, with \ensuremath{\chi} continuing to increase above the N\'eel antiferromagnetic ordering temperature (${T}_{\mathrm{N}}=70\phantom{\rule{0.16em}{0ex}}\mathrm{K}$), peaking at \ensuremath{\sim}250 K, then decreasing gently above. It is remarkable that this peak susceptibility temperature corresponds to the onset of anisotropic negative thermal expansion in both the $a$ and $c$ axes, suggesting that magnetic interactions are affecting the structure even well above the N\'eel point. A systematic investigation into local bonding correlations, from time-of-flight neutron pair distribution function analyses, shows the octahedral volume around each Fe site growing monotonically while adjacent octahedra tilt toward one another before relaxing away past this peak in the anomalous magnetic susceptibility. We use inelastic-neutron scattering to map spin-wave excitations in FeAs at temperatures above and below the ${T}_{\mathrm{N}}$. We find magnetic excitations near ${T}_{\mathrm{N}}$ to be very different from the excitations in the ground state at 1.5 K. Spin waves measured at 1.5 K are three dimensional (3D), however, in the vicinity of the magnetic transition, the magnetic fluctuations clearly indicate two-dimensional (2D) character in this intrinsically 3D crystal structure. Unlike the undoped 2D parents of iron-arsenide superconductors, where the magnetic correlations are considerably weaker along the $c$ axis than in the $\mathit{ab}$ plane, inelastic neutron scattering here shows that the spin fluctuations in the 3D FeAs binary are nearly 2D in the $\mathit{bc}$ plane at 90 K. These results demonstrate the importance of short-range correlations in understanding the magnetic properties of transition-metal binaries, and suggest how 2D excitations, even in a 3D structure, can potentially become a breeding ground for unconventional superconductivity.

Electron Doping of the Iron-Arsenide Superconductor CeFeAsO Controlled by Hydrostatic Pressure.

In the iron-pnictide material CeFeAsO not only the Fe moments, but also the local 4f moments of the Ce order antiferromagnetically at low temperatures. We elucidate on the peculiar role of the Ce on the emergence of superconductivity. While application of pressure suppresses the iron SDW ordering temperature monotonously up to 4GPa, the Ce-4f magnetism is stabilized until both types of magnetic orders disappear abruptly and a narrow SC dome develops. With further increasing pressure characteristics of a Kondo-lattice system become more and more apparent in the electrical resistivity. This suggests a connection of the emergence of superconductivity with the extinction of the magnetic order and the onset of Kondo screening of the Ce-4f moments.

Superconductivity-induced transverse plasma mode and phonon anomaly in the c -axis response of the bilayer compound RbCa2Fe4As4F2

With infrared spectroscopy we studied the out-of-plane ($c$-axis) response of the iron arsenide superconductor ACa$_2$Fe$_4$As$_4$F$_2$ (A = Rb,Cs) which has a bilayer structure similar to the high $T_c$ cuprates YBa$_2$Cu$_3$O$_7$ (YBCO) and Bi$_2$Sr$_2$CaCu$_2$O$_8$ (Bi2212). In analogy to the cuprates, we observe a superconductivity-induced transverse plasma mode (tPM) and a phonon anomaly that are both signatures of local electric field effects that arise from a large difference between the local conductivities in the intra- and inter-bilayer regions. Using a multilayer model developed for the cuprates, we obtain a good description of the $c$-axis response and derive the local conductivities at $T \simeq T_c$ of $\sigma_1^{\mathrm{bl}}(\omega \rightarrow 0) \simeq$ 1\,000 $\Omega^{-1}\mathrm{cm}^{-1}$ and $\sigma_1^{\mathrm{int}}(\omega \rightarrow 0) \simeq$ 15 $\Omega^{-1}\mathrm{cm}^{-1}$, respectively, that are similar to the ones previously found in underdoped YBCO. Different from the cuprates, we find no evidence of a normal state pseudogap in terms of a partial suppression of the low-energy electronic states that sets in already well above $T_c$. There is also no clear sign of an onset of precursor superconducting pairing correlations well above $T_c \simeq$ 30~K. This highlights that the pseudogap and the precursor superconducting pairing well above $T_c$ are unique features of the cuprates with their strong electronic correlations and, for example, not just the result of a strongly anisotropic electronic response due to the layered crystal structure.

NMR and NQR studies on transition-metal arsenide superconductors LaRu2As2, KCa2Fe4As4F2, and A2Cr3As3**Project supported by the National Natural Science Foundation of China (Grant Nos. 11674377, 11634015, and 11974405), the National Key R&D Program of China (Grant Nos. 2017YFA0302904 and 2016YFA0300502), and J. Y. also acknowledges support by the Youth Innovation Promotion Association of Chinese Academy of Sciences.

We report 75As-nuclear magnetic resonance (NMR) and nuclear quadrupole resonance (NQR) measurements on transition-metal arsenides LaRu2As 2, KCa2Fe4As4F2, and A2Cr3As3. In the superconducting state of LaRu2As2, a Hebel–Slichter coherence peak is found in the temperature dependence of the spin-lattice relaxation rate 1/T1 just below Tc, which indicates that LaRu2As2 is a full-gap superperconducor. For KCa2Fe4As4F2, antiferromagnetic spin fluctuations are observed in the normal state. We further find that the anisotropy rate is small and temperature independent, implying that the low energy spin fluctuations are isotropic in spin space. Our results indicate that KCa2Fe4As4F2 is a moderately overdoped iron-arsenide high-temperature superconductor with a stoichiometric composition. For A2Cr3As3 (A = Na, K, Rb, Cs), we calculate the electric field gradient by first-principle method and assign the 75As-NQR peaks to two crystallographically different As sites, paving the way for further NMR investigation.

Dictionary learning in Fourier-transform scanning tunneling spectroscopy

Modern high-resolution microscopes are commonly used to study specimens that have dense and aperiodic spatial structure. Extracting meaningful information from images obtained from such microscopes remains a formidable challenge. Fourier analysis is commonly used to analyze the structure of such images. However, the Fourier transform fundamentally suffers from severe phase noise when applied to aperiodic images. Here, we report the development of an algorithm based on nonconvex optimization that directly uncovers the fundamental motifs present in a real-space image. Apart from being quantitatively superior to traditional Fourier analysis, we show that this algorithm also uncovers phase sensitive information about the underlying motif structure. We demonstrate its usefulness by studying scanning tunneling microscopy images of a Co-doped iron arsenide superconductor and prove that the application of the algorithm allows for the complete recovery of quasiparticle interference in this material.

Optical Signature of a Crossover from Mott- to Slater-Type Gap in Sr2Ir1−xRhxO4

With optical spectroscopy we provide evidence that the insulator-metal transition in Sr_{2}Ir_{1-x}Rh_{x}O_{4} occurs close to a crossover from the Mott- to the Slater-type. The Mott gap at x=0 persists to high temperature and evolves without an anomaly across the Néel temperature, T_{N}. Upon Rh doping, it collapses rather rapidly and vanishes around x=0.055. Notably, just as the Mott gap vanishes yet another gap appears that is of the Slater-type and develops right below T_{N}. This Slater gap is only partial and is accompanied by a reduced scattering rate of the remaining free carriers, similar as in the parent compounds of the iron arsenide superconductors.

Lattice disorder effect on magnetic ordering of iron arsenides

This study investigates magnetic ordering temperature in nano- and mesoscale structural features in an iron arsenide. Although magnetic ground states in quantum materials can be theoretically predicted from known crystal structures and chemical compositions, the ordering temperature is harder to pinpoint due to potential local lattice variations that calculations may not account for. In this work we find surprisingly that a locally disordered material can exhibit a significantly larger Néel temperature (TN) than an ordered material of precisely the same chemical stoichiometry. Here, a EuFe2As2 crystal, which is a ‘122’ parent of iron arsenide superconductors, is found through synthesis to have ordering below TN = 195 K (for the locally disordered crystal) or TN = 175 K (for the ordered crystal). In the higher TN crystals, there are shorter planar Fe-Fe bonds [2.7692(2) Å vs. 2.7745(3) Å], a randomized in-plane defect structure, and diffuse scattering along the [00 L] crystallographic direction that manifests as a rather broad specific heat peak. For the lower TN crystals, the a-lattice parameter is larger and the in-plane microscopic structure shows defect ordering along the antiphase boundaries, giving a larger TN and a higher superconducting temperature (Tc) upon the application of pressure. First-principles calculations find a strong interaction between c-axis strain and interlayer magnetic coupling, but little impact of planar strain on the magnetic order. Neutron single-crystal diffraction shows that the low-temperature magnetic phase transition due to localized Eu moments is not lattice or disorder sensitive, unlike the higher-temperature Fe sublattice ordering. This study demonstrates a higher magnetic ordering point arising from local disorder in 122.

Nanoscale interlayer defects in iron arsenides

Using a local real-space microscopy probe, we discover evidence of nanoscale interlayer defects along the c-crystallographic direction in BaFe2As2 (‘122’) based iron-arsenide superconductors. We find ordered 122 atomic arrangements within the ab-plane, and within regions of ~10 to 20 nm size perpendicular to this plane. While the FeAs substructure is very rigid, Ba ions are relatively weakly bound and can be displaced from the 122, forming stacking faults resulting in the physical separation of the 122 between adjacent ordered domains. The evidence for interlayer defects between the FeAs superconducting planes gives perspective on the minimal connection between interlayer chemical disorder and high-temperature superconductivity. In particular, the Cooper pairs may be finding a way around such localized interlayer defects through a percolative path of the ordered layered 122 lattice that may not affect Tc.

Strong electron-boson coupling in the iron-based superconductor BaFe1.9Pt0.1As2 revealed by infrared spectroscopy

Understanding the formation of Cooper pairs in iron-based superconductors is one of the most important topics in condensed matter physics. In conventional superconductors, the electron-phonon interaction leads to the formation of Cooper pairs. In conventional strong-coupling superconductors like lead (Pb), the features due to electron-phonon interaction are evident in the infrared absorption spectra. Here we investigate the infrared absorption spectra of the iron arsenide superconductor BaFe1.9Pt0.1As2. We find that this superconductor has fully gapped (nodeless) Fermi surfaces, and we observe the strong-coupling electron-boson interaction features in the infrared absorption spectra. Through modeling with the Eliashberg function based on Eliashberg theory, we obtain a good quantitative description of the energy gaps and the strong-coupling features. The full Eliashberg equations are solved to check the self-consistency of the electron-boson coupling spectrum, the largest energy gap, and the transition temperature (Tc). Our experimental data and analysis provide compelling evidence that superconductivity in BaFe1.9Pt0.1As2 is induced by the coupling of electrons to a low-energy bosonic mode that does not originate solely from phonons.

Antiferromagnetic order in CaK(Fe1−xNix)4As4 and its interplay with superconductivity

The magnetic order in CaK(Fe[1-x]Ni[x])4As4 (1144) single crystals (x = 0.051 and 0.033) has been studied by neutron diffraction. We observe magnetic Bragg peaks associated to the same propagation vectors as found for the collinear stripe antiferromagnetic (AFM) order in the related BaFe2As2 (122) compound. The AFM state in 1144 preserves tetragonal symmetry and only a commensurate, non-collinear structure with a hedgehog spin-vortex crystal (SVC) arrangement in the Fe plane and simple AFM stacking along the c direction is consistent with our observations. The SVC order is promoted by the reduced symmetry in the FeAs layer in the 1144 structure. The long-range SVC order coexists with superconductivity, however, similar to the doped 122 compounds, the ordered magnetic moment is gradually suppressed with the developing superconducting order parameter. This supports the notion that both collinear and non-collinear magnetism and superconductivity are competing for the same electrons coupled by Fermi surface nesting in iron arsenide superconductors.

High-pressure effects on isotropic superconductivity in the iron-free layered pnictide superconductor BaPd2As2

While the layered 122 iron arsenide superconductors are highly anisotropic, unconventional, and exhibit several forms of electronic orders that coexist or compete with superconductivity in different regions of their phase diagrams, we find in the absence of iron in the structure that the superconducting characteristics of the end member BaPd2As2 are surprisingly conventional. Here we report on complementary measurements of specific heat, magnetic susceptibility, resistivity measurements, Andreev spectroscopy, and synchrotron high pressure x-ray diffraction measurements supplemented with theoretical calculations for BaPd2As2. Its superconducting properties are completely isotropic as demonstrated by the critical fields, which do not depend on the direction of the applied field. Under the application of high pressure, Tc is linearly suppressed, which is the typical behavior of classical phonon-mediated superconductors with some additional effect of a pressure-induced decrease in the electronic density of states and the electron-phonon coupling parameters. Structural changes in the layered BaPd2As2 have been studied by means of angle-dispersive diffraction in a diamond-anvil cell. At 12 GPa and 24.2 GPa we observed pressure induced lattice distortions manifesting as the discontinuity and, hence discontinuity in the Birch-Murnaghan equation of state. The bulk modulus is B0=40(6) GPa below 12 GPa and B0=142(3) GPa below 27.2 GPa.

CsMn4As3: A Layered Tetragonal Transition-Metal Pnictide Compound with an Antiferromagnetic Ground State.

We report the synthesis and properties of a new layered tetragonal ternary compound CsMn4As3 (structure type, KCu4S3; space group, P4/ mmm, no. 123; and Z = 2). The material is a small band gap semiconductor and exhibits an antiferromagnetic ground state associated with Mn spins. The compound exhibits a signature of a distinct magnetic moment canting event at 150(5) K with a canting angle ≈ 0.3°. Although some features of the magnetic characteristics of this new compound are qualitatively similar to those of the related BaMn2As2, the underlying Mn sublattices of the two materials are quite different. While the Mn square-lattice layers in BaMn2As2 are equally spaced along the c-direction with the interlayer distance dLBa = 6.7341(4) Å, the Mn sublattice forms bilayers in CsMn4As3 with the interlayer distance within a bilayer being dLCs = 3.1661(6) Å; the distance between the two adjacent bilayers is dB = 7.290(6) Å. This difference in the Mn sublattice is bound to significantly alter the energy balance among the J1, J2, and J c exchange interactions within the J1- J2- J c model compared to those in BaMn2As2 and the other related 122 compounds, including the well-known iron-arsenide superconductor parent compound BaFe2As2. Owing to the novelty of its transition-metal sublattice, this new addition to the family of tetragonal materials related to the iron-based superconductors brings prospects for doping and pressure studies in the search of new superconducting phases as well as other exciting correlated electron properties.

Correlation between non-Fermi-liquid behavior and superconductivity in (Ca, La)(Fe,Co) As2 iron arsenides: A high-pressure study

Non-Fermi-liquid (NFL) phenomena associated with correlation effects have been widely observed in the phase diagrams of unconventional superconducting families. Exploration of the correlation between the normal state NFL, regardless of its microscopic origins, and the superconductivity has been argued as a key to unveiling the mystery of the high-Tc pairing mechanism. Here we systematically investigate the pressure-dependent in-plane resistivity and Hall coefficient (RH ) of a high-quality 112-type Fe-based superconductor Ca1-xLaxFe1-yCoyAs2 (x = 0.2,y = 0.02). With increasing pressure, the normal-state resistivity of the studied sample exhibits a pronounced crossover from non-Fermi-liquid to Fermi-liquid behaviors. Accompanied with this crossover, Tc is gradually suppressed. In parallel, the extremum in the Hall coefficient RH (T ) curve, possibly due to anisotropic scattering induced by spin fluctuations, is also gradually suppressed. The symbiosis of NFL and superconductivity implies that these two phenomena are intimately related. Further study on the pressure-dependent upper critical field reveals that the two-band effects are also gradually weakened with increasing pressure and reduced to the one-band Werthamer-Helfand-Hohenberg limit in the low-Tc regime. Overall, our paper supports the picture that NFL, multigap, and extreme RH (T ) are all of the same magnetic origin, i.e., the spin fluctuations in the 112 iron arsenide superconductors.

Local Orthorhombicity in the Magnetic C_{4} Phase of the Hole-Doped Iron-Arsenide Superconductor Sr_{1-x}Na_{x}Fe_{2}As_{2}.

We report on temperature-dependent pair distribution function measurements of Sr_{1-x}Na_{x}Fe_{2}As_{2}, an iron-based superconductor system that contains a magnetic phase with reentrant tetragonal symmetry, known as the magnetic C_{4} phase. Quantitative refinements indicate that the instantaneous local structure in the C_{4} phase comprises fluctuating orthorhombic regions with a length scale of ∼2 nm, despite the tetragonal symmetry of the average static structure. Additionally, local orthorhombic fluctuations exist on a similar length scale at temperatures well into the paramagnetic tetragonal phase. These results highlight the exceptionally large nematic susceptibility of iron-based superconductors and have significant implications for the magnetic C_{4} phase and the neighboring C_{2} and superconducting phases.

Two-Dimensional Massless Dirac Fermions in Antiferromagnetic AFe_{2}As_{2} (A=Ba,Sr).

We report infrared studies of AFe_{2}As_{2} (A=Ba, Sr), two representative parent compounds of iron-arsenide superconductors, at magnetic fields (B) up to 17.5T. Optical transitions between Landau levels (LLs) wereobserved in the antiferromagnetic states of these two parent compounds. Our observation of a sqrt[B] dependence of the LL transition energies, the zero-energy intercepts at B=0 T under the linear extrapolations of the transition energies and the energy ratio (∼2.4) between the observed LL transitions, combined with the linear band dispersions in two-dimensional (2D) momentum space obtained by theoretical calculations, demonstrates the existence of massless Dirac fermions in the antiferromagnet BaFe_{2}As_{2}. More importantly, the observed dominance of the zeroth-LL-related absorption features and the calculated bands with extremely weak dispersions along the momentum direction k_{z} indicate that massless Dirac fermions in BaFe_{2}As_{2} are 2D. Furthermore, we find that the total substitution of the barium atoms in BaFe_{2}As_{2} by strontium atoms not only maintains 2D massless Dirac fermions in this system, but also enhances their Fermi velocity, which supports that the Dirac points in iron-arsenide parent compounds are topologically protected.

Pressure-induced transition to the collapsed tetragonal phase in BaCr2As2

The structural and electronic properties of $\mathrm{BaC}{\mathrm{r}}_{2}\mathrm{A}{\mathrm{s}}_{2}$, which is isostructural to the 122 iron arsenide superconductors, are studied at high pressures using synchrotron x-ray powder diffraction, electrical resistivity measurements, and first-principles calculations. At a pressure of about 18.5 GPa, an isostructural phase transition to a collapsed tetragonal phase is observed, similar to that in $\mathrm{BaF}{\mathrm{e}}_{2}\mathrm{A}{\mathrm{s}}_{2}$. In both phases, $\mathrm{BaC}{\mathrm{r}}_{2}\mathrm{A}{\mathrm{s}}_{2}$ is a normal metal. Electronic structure calculations suggest a metallic and antiferromagnetic ground state with $G$-type magnetic order for the collapsed tetragonal phase.

Various Arsenic Network Structures in 112-Type Ca1–xLaxFe1–yPdyAs2 Revealed by Synchrotron X-ray Diffraction Experiments

Two novel 112-type palladium-doped iron arsenides were synthesized and identified using comprehensive studies involving synchrotron X-ray diffraction and X-ray absorption near-edge structure (XANES) experiments. Whereas in-plane arsenic zigzag chains were found in the 112-type superconducting iron arsenide Ca1-xLaxFeAs2 with maximum Tc = 34 K, deformed arsenic network structures appeared in other 112-type materials, such as longitudinal arsenic zigzag chains in CaFe1-yPdyAs2 (y ∼ 0.51) and arsenic square sheets constructed via hypervalent bonding in Ca1-xLaxFe1-yPdyAs2 (x ∼ 0.31, y ∼ 0.30). As K-edge XANES spectra clarified the similar oxidization states around FeAs4 tetrahedrons, alluding to possible parents for high-Tc 112-type iron arsenide superconductors.

Iron arsenide superconductors (CaFeAs)10MnAs8 with metallic interlayers (M = Pt, Pd; n = 3, 4)

The compounds referred to as 1038 and 1048 phases (CaFeAs)10PtnAs8 (n = 3,4) are the structurally most complex iron arsenide superconductors and the first examples with metallic interlayers. The electronic subsystems of FeAs and PtnAs8 layers hardly interact and the contribution of the metallic PtnAs8 interlayers to the Fermi surface is so small that the typical nesting is not degraded. (CaFeAs)10Pt3As8 is the parent compound of the 1038/1048 materials which undergoes the typical magneto‐structural phase transition in spite of the already triclinic lattice. Superconductivity is controlled by the same doping mechanisms as known from simpler FeAs systems. High critical temperatures up to 38 K occur in both 1038 and 1048 phases if the FeAs layers are clean (free from Pt) and electron doped by charge transfer either from Pt4As8 in 1048 or by rare‐earth doping of the calcium layer in 1038 compounds. The presence of two negatively charged layers (FeAs)δ− and (PtnAs8)δ− which compete for the electrons transferred from the Ca2+ ions is unique in the family of iron arsenide superconductors. Geometric incompatibilities of the FeAs and PtnAs8 slabs cause severe stacking disorder. The robustness of superconductivity against low lattice symmetry and significant structural imperfection of the interlayer is quite remarkable and underlines that the FeAs slabs are the key in controlling and understanding high‐temperature superconductivity in iron arsenides.Crystal structure of (CaFeAs)10Pt3As8 and the Pt3As8 layer.

Doping evolution of the superconducting gap structure in the underdoped iron arsenideBa1−xKxFe2As2revealed by thermal conductivity

The thermal conductivity kappa of the iron-arsenide superconductor Ba1-xKxFe2As2 was measured for heat currents parallel and perpendicular to the tetragonal c axis at temperatures down to 50 mK and in magnetic fields up to 15 T. Measurements were performed on samples with compositions ranging from optimal doping (x = 0.34; Tc = 39 K) down to dopings deep into the region where antiferromagnetic order coexists with superconductivity (x = 0.16; Tc = 7 K). In zero field, there is no residual linear term in kappa(T) as T goes to 0 at any doping, whether for in-plane or inter-plane transport. This shows that there are no nodes in the superconducting gap. However, as x decreases into the range of coexistence with antiferromagnetism, the residual linear term grows more and more rapidly with applied magnetic field. This shows that the superconducting energy gap develops minima at certain locations on the Fermi surface and these minima deepen with decreasing x. We propose that the minima in the gap structure arise when the Fermi surface of Ba1-xKxFe2As2 is reconstructed by the antiferromagnetic order.

Expansion of the tetragonal magnetic phase with pressure in the iron arsenide superconductorBa1−xKxFe2As2

In the temperature-concentration phase diagram of most iron-based superconductors, antiferromagnetic order is gradually suppressed to zero at a critical point, and a dome of superconductivity forms around that point. The nature of the magnetic phase and its fluctuations is of fundamental importance for elucidating the pairing mechanism. In Ba{1-x}KxFe2As2 and Ba{1-x}NaxFe2As2, it has recently become clear that the usual stripe-like magnetic phase, of orthorhombic symmetry, gives way to a second magnetic phase, of tetragonal symmetry, near the critical point, between x = 0.24 and x = 0.28. Here we report measurements of the electrical resistivity of Ba{1-x}KxFe2As2 under applied hydrostatic pressures up to 2.75 GPa, for x = 0.22, 0.24 and 0.28. We track the onset of the tetragonal magnetic phase using the sharp anomaly it produces in the resistivity. In the temperature-concentration phase diagram of Ba{1-x}KxFe2As2, we find that pressure greatly expands the tetragonal magnetic phase, while the stripe-like phase shrinks. This raises the interesting possibility that the fluctuations of the former phase might be involved in the pairing mechanism responsible for the superconductivity.