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The electronic structure, lattice dynamics, and electron-phonon coupling (EPC) of the newly discovered (Ba,K)SbO$_3$ superconductors are investigated by first-principles calculations. The EPC of (Ba,K)SbO$_3$ is significantly enhanced by considering non-local electronic correlation using the Heyd-Scuseria-Ernzerhof hybrid exchange-correlation functional (HSE06). The EPC strength {\lambda} of Ba$_{0.35}$K$_{0.65}$SbO$_3$ is strongly increased from 0.33 in local-density approximation calculations to 0.59 in HSE06 calculations, resulting in a superconducting transition temperature Tc of about 14.9 K, which is in excellent agreement with experimental value of ~ 15 K. Our findings suggest (Ba,K)SbO$_3$ are extraordinary conventional superconductors, where non-local electronic correlation expands the bandwidth, enhances the EPC, and boosts the Tc. Moreover, we find both {\lambda} and Tc depend crucially on the K-doping level for (Ba,K)SbO$_3$ and (Ba,K)SbO$_3$ compounds. (Ba,K)SbO$_3$ have stronger EPC strength and higher Tc than those of (Ba,K)SbO$_3$ at the same K-doping level., Comment: 29 pages, 10 figures

Superconducting bismuthates (Ba,K)BiO$_{3}$ (BKBO) constitute an interesting class of superconductors in that superconductivity with a remarkably high $T_\mathrm{c}$ of 30 K arises in proximity to charge density wave (CDW) order. Prior understanding on the driving mechanism of the CDW and superconductivity emphasizes the role of either bismuth (negative $U$ model) or oxygen ions (ligand hole model). While holes in BKBO presumably reside on oxygen owing to their negative charge transfer energy, so far there has been no other comparative material studied. Here, we introduce (Ba,K)SbO$_{3}$ (BKSO) in which the Sb 5$s$ orbital energy is higher than that of the Bi 6$s$ orbitals enabling tuning of the charge transfer energy from negative to slightly positive. The parent compound BaSbO$_{3-\delta}$ shows a larger CDW gap compared to the undoped bismuthate BaBiO$_{3}$. As the CDW order is suppressed via potassium substitution up to 65 %, superconductivity emerges, rising up to $T_\mathrm{c}$ = 15 K. This value is lower than the maximum $T_\mathrm{c}$ of BKBO, but higher by more than a factor of two at comparable potassium concentrations. The discovery of an enhanced CDW gap and superconductivity in BKSO indicates that the sign of the charge transfer energy may not be crucial, but instead strong metal-oxygen covalency plays the essential role in constituting a CDW and high-$T_\mathrm{c}$ superconductivity in the main-group perovskite oxides.

The most effective way to enhance the dissipation-free supercurrent in presence of magnetic field for type II superconductors is the introduction of defects that acts as artificial pinning centres (APCs) for the vortices. For instance, the in-field critical current density of doped BaFe2As2 (Ba122), one of the most technologically important Fe-based superconductors, has been improved over the last decade by APCs created by ion-irradiation. The technique of ion-irradiation has been commonly implemented to determine the ultimate superconducting properties. However, this method is rather complicated and expensive. Here, we report on a surprisingly high critical current density and strong pinning efficiency close to the crystallographic c-axis for a K-doped Ba122 epitaxial thin film without APCs, achieving performance comparable to ion-irradiated K-doped Ba122 single crystals. Microstructural analysis reveals that the film is composed of columnar grains having width around 30-60 nm. The grains are rotated around the b- (or a-) axis by 1.5 degree and around the c-axis by -1 degree, resulting in the formation of low-angle grain boundary networks. This study demonstrates that the upper limit of in-field properties reached in ion-irradiated K-doped Ba122 is achievable by grain boundary engineering, which is a simple and industrially scalable manner., Comment: Main text with Supplement Material

Perpendicular magnetic anisotropy of the new ferromagnetic semiconductor (Ba,K)(Zn,Mn)$_{2}$As$_{2}$ is studied by angle-dependent x-ray magnetic circular dichroism measurements. The large magnetic anisotropy with the anisotropy field of 0.85 T is deduced by fitting the Stoner-Wohlfarth model to the magnetic-field-angle dependence of the projected magnetic moment. Transverse XMCD spectra highlights the anisotropic distribution of Mn 3$d$ electrons, where the $d_{xz}$ and $d_{yz}$ orbitals are less populated than the $d_{xy}$ state because of the $D_{2d}$ splitting arising from the elongated MnAs$_{4}$ tetrahedra. It is suggested that the magnetic anisotropy originates from the degeneracy lifting of $p$-$d_{xz}$, $d_{yz}$ hybridized states at the Fermi level and resulting energy gain due to spin-orbit coupling when spins are aligned along the $z$ direction.

In-plane anisotropy of electrical resistivity was studied in samples of the hole-doped Ba$_{1-x}$K$_x$Fe$_2$As$_2$ in the composition range $0.21 \leq x \leq 0.26$ where anisotropy changes sign. Low-temperature ($\sim$20~K) irradiation with relativistic 2.5 MeV electrons was used to control the level of disorder and residual resistivity of the samples. Modification of the stress-detwinning technique enabled measurements of the same samples before and after irradiation, leading to conclusion of anisotropic character of predominantly inelastic scattering processes. Our main finding is that the resistivity anisotropy is of the same sign irrespective of residual resistivity, and remains the same in the orthorhombic $C_2$ phase above the re-entrant tetragonal transition. Unusual $T$-linear dependence of the anisotropy $\Delta \rho \equiv \rho_a(T)-\rho_b(T)$ is found in pristine samples with $x=$0.213 and $x=$0.219, without similar signatures in either $\rho_a(T)$ or $\rho_b(T)$. We show that this feature can be reproduced by a phenomenological model of R.~M.~Fernandes {\it et al.} Phys. Rev. Lett. {\bf 107},217002 (2011). We speculate that onset of fluctuations of nematic order on approaching the instability towards the re-entrant tetragonal phase contributes to this unusual dependence.

As-Based Zintl compounds Ba1-xKxCd2As2 crystallized in the CaAl2Si2-type structure (space group P3-m1) were prepared using solid-state reactions followed by hot-pressing. We have successfully substituted K for Ba up to x = 0.08, producing hole-carrier doping with concentrations up to 1.60*1020 cm-3. We have determined the band-gap value of non-doped BaCd2As2 to be 0.40 eV from the temperature dependence of the electrical resistivity. Both the electrical resistivity and the Seebeck coefficient decrease with hole doping, leading to a power factor value of 1.28 mW m-1 K-2 at 762 K for x = 0.04. A first-principles band calculation shows that the relatively large power factor mainly originates from the two-fold degeneracy of the bands comprising As px,y orbitals and from the anisotropic band structure at the valence-band maximum. The lattice thermal conductivity is suppressed by the K doping to 0.46 W m-1 K-1 at 773 K for x = 0.08, presumably due to randomness. The effect of randomness is compensated by an increase in the electronic thermal conductivity, which keeps the total thermal conductivity approximately constant. In consequence, the dimensionless figure-of-merit ZT reaches a maximum value of 0.81 at 762 K for x = 0.04., Comment: 7 pages, 9 figures

(Ba,K)Fe2As2 superconducting wires and tapes are fabricated by using hot isostatic pressing (HIP) technique, and their superconducting properties are studied. In the HIP round wire, transport critical current density (Jc) at 4.2 K has achieved record-high value of 175 kA/cm2 at zero field, and exceeds 20 kA/cm2 even at 100 kOe. Improvement of polycrystalline powder synthesis may play a key role for the enhancement of Jc. In the HIP tape, even larger transport Jc of 380 kA/cm2 is realized at zero field. Based on magnetization and magneto-optical measurements, possible further enhancement of Jc is discussed., Comment: 16 pages, 6 figures

We have studied the atomic and magnetic structure of the dilute ferromagnetic semiconductor system (Ba,K)(Zn,Mn)$_2$As$_2$ through atomic and magnetic pair distribution function analysis of temperature-dependent x-ray and neutron total scattering data. We detected a change in curvature of the temperature-dependent unit cell volume of the average tetragonal crystallographic structure at a temperature coinciding with the onset of ferromagnetic order. We also observed the existence of a well-defined local orthorhombic structure on a short length scale of $\lesssim 5$ \AA, resulting in a rather asymmetrical local environment of the Mn and As ions. Finally, the magnetic PDF revealed ferromagnetic alignment of Mn spins along the crystallographic $c$-axis, with robust nearest-neighbor ferromagnetic correlations that exist even above the ferromagnetic ordering temperature. We discuss these results in the context of other experiments and theoretical studies on this system.

Using four different experimental techniques, we performed comprehensive studies of the bulk superconductive properties of single crystals of the nearly optimally doped $Ba_{1-x}K_xFe_2As_2$ ($T_{c} \approx 36\,K$), a typical representative of the 122 family. We investigated temperature dependencies of the (i) specific heat $C_{el}(T)$, (ii) first critical magnetic field $H_{c1}(T)$, (iii) intrinsic multiple Andreev reflection effect (IMARE), and (iv) infrared reflectivity spectra. All data clearly show the presence of (at least) two superconducting nodeless gaps. The quantitative data on the superconducting spectrum obtained by four different techniques are consistent with each other: (a) the small energy gap $\Delta_S(0) \approx 1.8 - 2.5\,meV$, and the large gap energy $\Delta_L(0) \approx 9.5 - 11.3\,meV$ that demonstrates the signature of an extended s-wave symmetry ($\sim~33 \%$ in-plane anisotropy), (b) the characteristic ratio $2\Delta_L/k_BT_C$ noticeably exceeds the BCS value., Comment: 16 pages, 9 figures

Strong pinning depends on the pinning force strength and number density of effective defects. Using hydrostatic pressure method, we demonstrate that hydrostatic pressure up to 1.2 GPa can significantly enhance flux pinning or Jc by a factor of up to 5 especially in both low and high fields in optimally doped Ba0.6K0.4Fe2As2 crystals. Our analysis on the flux pining mechanism indicate that both pinning centre number density (Np) and pinning force (Fp) are greatly increased by the pressure and contribute to strong pinning., Comment: Nil

We demonstrate a large enhancement of critical current density (Jc) up to 1.0x10^7 A/cm2 at 5 K under self-field in (Ba,K)Fe2As2 single crystals by irradiating 320 MeV Au ions. With the very promising potential of this material in mind, we have fabricated a (Ba,K)Fe2As2 superconducting wire through a powder-in-tube method combined with the hot isostatic pressing technique, whose effectiveness has been proven in industrial Bi2223 tapes. The Jc in the wire at 4.2 K has reached 37 kA/cm2 under self-field and 3.0 kA/cm2 at 90 kOe. Magneto-optical imaging of the wire confirmed the large intergranular Jc in the wire core., Comment: 20 pages, 5 figures, accepted for publication in Appl. Phys. Express

Resistivity Rho(T), Hall coefficient RH(T), superconducting transition temperature Tc and slopes of the upper critical field dHc2/dT were studied in (Ba1-xKx)Fe2As2 (x = 0.218, 0.356, 0.531) single crystals irradiated with fast neutrons. It is found that dTc/dRhoSC - the rate of decreasing Tc as a function of the RhoSC (RHoSC is the resistivity at T = Tc) - linearly increases with concentration x. Slow changes in the Hall coefficient RH, as well as the quadratic electronic contribution to the resistivity, show that there are no substantial changes in the topology of the Fermi surface caused by irradiation. The slopes of the upper critical field dHc2/dT in ab- and c-directions as a function of RHoSC determined by Hall measurements show a reasonable agreement with a model that suggests constancy of the band parameters., Comment: 6 pages, 8 figures

We report that high transport critical current density exceeding 104 A/cm2 at 4.2 K and 10 T can be obtained with good reproducibility for Ag sheathed (Ba,K)Fe2As2 (Ba 122) tapes by modifying the ex-situ powder-in-tube (PIT) method. The process involves cycles of the cold deformation and subsequent heat treatment. The intermediate cycles of flat rolling and heat treatment produce uniform fine-grained structure, resulting in an enhancement of transport Jc in applied magnetic fields. However, the rolled tapes contain cracks running traverse to the tape axis, which still limit the current pass along the tape axis. We found that the application of uniaxial pressing with small reduction rate at the final stage is very effective to heal those cracks, resulting in an extraordinary increase of the transport Jc. We achieved the highest Jc (at 4.2 K and 10 T) of 2.1x104 A/cm2 among the PIT processed Fe based wires and tapes reported so far. The Jc-H curves measured at higher temperatures maintains a small filed dependence up to around 20 K, suggesting that the tapes are promising for applications at higher temperatures as well as in liquid helium.

We found that the transport Jc of the ex-situ PIT processed (Ba,K)Fe2As2 (Ba-122) wire with single Ag sheath can be significantly enhanced by repeating the combined process of rolling and heat treatment. The transport Jc (4.2 K and 10 T) of 4.4 x 103 A/cm2 (Ic =15.7 A) was obtained for a thin tape of 0.3 mm in thickness, which is the highest value reported so far for the PIT processed 122 wires and tapes with a Ag sheath and processed by a conventional route. The measurement by a hybrid magnet showed that Jc-H curve maintains very small field dependence up to the strong magnetic field of 28 T as expected from the previously reported high Hc2 value. The core of the thin tape shows dense grain structure with less cracks and voids and indicates the development of c-axis alignment, although it is still incomplete. The researches to elucidate the origin of Jc enhancement and to have further improvement of transport Jc are now ongoing. The process is simple using a Ag single sheath and, therefore, more realistic technique for long length wire production., Comment: 8 pages, 7 figures

We report that single crystals of (Ba,K)Fe2As2 with Tc = 32 K have a pinning potential, U0, as high as 10^4 K, with U0 showing very little field depend-ence. In addition, the (Ba,K)Fe2As2 single crystals become isotropic at low temperatures and high magnetic fields, resulting in a very rigid vortex lattice, even in fields very close to Hc2. The rigid vortices in the two dimensional (Ba,K)Fe2As2 distinguish this compound from 2D high Tc cuprate superconductors with 2D vortices, and make it being capable of cearrying very high critical current.Flux jumping due to high Jc was also observed in large samples at low temperatures., Comment: 4 pages, 7 figures. submitted

We have fabricated c-axis Josephson junctions on single crystals of (Ba,K)Fe2As2 by using Pb as the counter electrode in two geometries, planar and point contact. Junctions in both geometries show resistively shunted junction I-V curves below the Tc of the counter electrode. Microwave induced steps were observed in the I-V curves, and the critical currents are suppressed with an in-plane magnetic field in a manner consistent with the small junction limit. ICRN products of up to 0.3 mV have been observed in these junctions at 4.2 K. The observation of Josephson coupling along the c-axis between (Ba,K)Fe2As2 and a conventional superconductor suggests the existence of a s-wave superconducting order parameter in this class of iron pnictide superconductors., Comment: 16 pages and 3 figures

Measurements of magnetotransport and current-voltage (I-V) characteristics up to 9 T were used to investigate the vortex phase diagram of an under-doped Measurements of magnetotransport and current-voltage (I-V) characteristics up to 9 T were used to investigate the vortex phase diagram of an under-doped (Ba,K)Fe2As2 single crystal with Tc=26.2 K. It is found that the anisotropy ratio of the upper critical field Hc2 decreases from 4 to 2.8 with decreasing temperature from Tc to 24.8 K. Consistent with the vortex-glass theory, the I-V curves measured at H=9 T can be well scaled with the vortex-glass transition temperature of Tg=20.7 K and critical exponents z=4.1 and v=1. Analyses in different magnetic fields produced almost identical critical exponent values, with some variation in Tg, corroborating the existence of the vortex-glass transition in this under-doped (Ba,K)Fe2As2 single crystal up to 9 T. A vortex phase diagram is presented, based on the evolution of Tg and Hc2 with magnetic field., Comment: 23 pages, 7 figures. accepted in Phys. Rev. B

We report large transport critical current densities observed in Ag-added (Ba,K)Fe2As2 superconducting wires prepared by an ex-situ powder-in-tube (PIT) process. The wire has a simple composite structure sheathed only by Ag. A precursor bulk material prepared by a melting process was ground into powder and put into a Ag tube. The composite was then cold worked into a wire and heat treated at 850$^\circ$C for sintering. Transport critical current densities, Jc, at 4.2 K are 1.0\times104 A/cm2 (Ic = 60.7 A) in self field and 1.1\times103 A/cm2 (Ic = 6.6 A) in 10 T. These are the highest values reported so far for the Fe-based superconducting wires., Comment: in press for Appl. Phys. Express

We report that (Ba,K)Fe2As2 superconductor (a transition temperature, Tc = 38 K) shows inverse Iron isotope effect (-0.18) (the sample including the larger atomic weight of Fe depicts higher Tc). Measurements of both temperature dependent magnetization and resistivity reveal a clear inverse shift by systematic studies on Tc using three types of Fe-isotopes (Fe-54, natural Fe and Fe-57). This indicates the first evidence of the inverse isotope effect in high-Tc superconductors. This atomic mass dependence on Tc implies the exotic coupling mechanism., Comment: 12 pages, 6 figures

The nature of the pairing state in iron-based superconductors is the subject of much debate. Here we argue that in one material, the stoichiometric iron pnictide KFe2As2, there is overwhelming evidence for a d-wave pairing state, characterized by symmetry-imposed vertical line nodes in the superconducting gap. This evidence is reviewed, with a focus on thermal conductivity and the strong impact of impurity scattering on the critical temperature Tc. We then compare KFe2As2 to Ba0.6K0.4Fe2As2, obtained by Ba substitution, where the pairing symmetry is s-wave and the Tc is ten times higher. The transition from d-wave to s-wave within the same crystal structure provides a rare opportunity to investigate the connection between band structure and pairing mechanism. We also compare KFe2As2 to the nodal iron-based superconductor LaFePO, for which the pairing symmetry is probably not d-wave, but more likely s-wave with accidental line nodes.

The surprisingly rapid relaxation of the sustainable current density in the critical state of single crystalline Ba$_{1-x}$K$_{x}$Fe$_{2}$As$_{2}$ is investigated for magnetic fields oriented parallel to the c-axis and to the $ab$--plane respectively. Due to the inadequacy of standard analysis procedures developed for flux creep in the high temperature superconducting cuprates, we develop a simple, straightforward data treatment technique that reveals the creep mechanism and the creep exponent $\mu$. At low magnetic fields, below the second magnetization peak, $\mu$ varies only slightly as function of temperature and magnetic flux density $B$. From the data, we determine the temperature- and field dependence of the effective activation barrier for creep. At low temperatures, the measured current density approaches the zero--temperature critical current density (in the absence of creep) to within a factor 2, thus lending credence to earlier conclusions drawn with respect to the pinning mechanism. The comparable values of the experimental screening current density and the zero-temperature critical current density reveals the limited usefulness of the widely used "interpolation formula"., Comment: Physical Review B (2012) Accepted

We report measurements of quasiparticle relaxation dynamics in the high-temperature superconductor (Ba,K)Fe$_{2}$As$_{2}$ in optimally doped, underdoped and undoped regimes. In the underdoped sample, spin-density wave (SDW) order forms at $\sim$85 K, followed by superconductivity at $\sim$ 28 K. We find the emergence of a normal-state order that suppresses SDW at a temperature $T^{\ast} \sim$ 60 K and argue that this normal-state order is a precursor to superconductivity., Comment: Major revision

The relation between the spin-density-wave (SDW) and superconducting order is a central topic in current research on the FeAs-based high Tc superconductors. Conflicting results exist in the LaFeAs(O,F)-class of materials, for which whether the SDW and superconductivity are mutually exclusive or they can coexist has not been settled. Here we show that for the (Ba,K)Fe2As2 system, the SDW and superconductivity can coexist in an extended range of compositions. The availability of single crystalline samples and high value of the energy gaps would make the materials a model system to investigate the high Tc ferropnictide superconductivity., Comment: 4 pages, 5 figures

Superconductivity was recently observed in the iron-arsenic-based compounds with a superconducting transition temperature (Tc) as high as 56K [1-7], naturally raising comparisons with the high Tc copper oxides. The copper oxides have layered crystal structures with quasi-two-dimensional electronic properties, which led to speculations that reduced dimensionality (that is, extreme anisotropy) is a necessary prerequisite for superconductivity at temperatures above 40 K [8,9]. Early work on the iron-arsenic compounds seemed to support this view [7,10]. Here we report measurements of the electrical resistivity in single crystals of (Ba,K)Fe2As2 in a magnetic field up to 60 T. We find that the superconducting properties are in fact quite isotropic, being rather independent of the direction of the applied magnetic fields at low temperature. Such behaviour is strikingly different from all previously-known layered superconductors [9,11], and indicates that reduced dimensionality in these compounds is not a prerequisite for high-temperature superconductivity. We suggest that this situation arises because of the underlying electronic structure of the iron-arsenide compounds, which appears to be much more three dimensional than that of the copper oxides. Extrapolations of low-field single-crystal data incorrectly suggest a high anisotropy and a greatly exaggerated zero-temperature upper critical field., Comment: To appear in Nature

Directional point-contact Andreev-reflection spectroscopy measurements on the Ba$_{0.55}$K$_{0.45}$Fe$_2$As$_2$ single crystals are presented. The spectra show significant differences when measured in the $ab$ plane in comparison with those measured in the $c$ direction of the crystal. In the latter case only a reduced point-contact conductance around zero bias has been revealed persisting well above $T_c$ and probably related to the structural and magnetic transitions in the system. Within the $ab$ plane two superconducting energy gaps are detected below $T_c$. Here a reduced conductance above $T_c$ could also be found. The fits of the $ab$-plane data to the superconducting s-wave two-gap model indicate that the smaller gap has a size below the BCS value while the large gap reveals much higher coupling strength., Comment: published version

The recent discovery and subsequent developments of FeAs-based superconductors have presented novel challenges and opportunities in the quest for superconducting mechanisms in correlated-electron systems. Central issues of ongoing studies include interplay between superconductivity and magnetism as well as the nature of the pairing symmetry reflected in the superconducting energy gap. In the cuprate and RE(O,F)FeAs (RE = rare earth) systems, the superconducting phase appears without being accompanied by static magnetic order, except for narrow phase-separated regions at the border of phase boundaries. By muon spin relaxation measurements on single crystal specimens, here we show that superconductivity in the AFe$_{2}$As$_{2}$ (A = Ca,Ba,Sr) systems, in both the cases of composition and pressure tunings, coexists with a strong static magnetic order in a partial volume fraction. The superfluid response from the remaining paramagnetic volume fraction of (Ba$_{0.5}$K$_{0.5}$)Fe$_{2}$As$_{2}$ exhibits a nearly linear variation in T at low temperatures, suggesting an anisotropic energy gap with line nodes and/or multi-gap effects., Comment: 14 pages 7 figures (4 for main text and 3 for on-line supplementary documents)

Zero-field (ZF) muon spin relaxation ($\mu$SR) measurements have revealed static commensurate magnetic order of Fe moments in NdOFeAs below $T_{N} \sim 135$ K, with the ordered moment size nearly equal to that in LaOFeAs, and confirmed similar behavior in BaFe$_{2}$As$_{2}$. In single crystals of superconducting (Ba$_{0.55}$K$_{0.45}$)Fe$_{2}$As$_{2}$, $\mu$SR spectra indicate static magnetism with incommensurate or short-ranged spin structure in $\sim$ 70 % of volume below $T_{N} \sim$ 80 K, coexisting with remaining volume which exhibits superfluid-response consistent with nodeless gap below $T_{c}\sim 30$ K., Comment: 4 pages 4 figures

The de Gennes and Maki theory of gapless superconductivity for dirty superconductors is used to interpret the tunneling measurements on the strongly type-II high-Tc oxide-superconductor Ba1-xKxBiO3 in high magnetic fields up to 30 Tesla. We show that this theory is applicable at all temperatures and in a wide range of magnetic fields starting from 50 percent of the upper critical field Bc2. In this magnetic field range the measured superconducting density of states (DOS) has the simple energy dependence as predicted by de Gennes from which the temperature dependence of the pair-breaking parameter alpha(T), or Bc2(T), has been obtained. The deduced temperature dependence of Bc2(T) follows the Werthamer-Helfand-Hohenberg prediction for classical type-II superconductors in agreement with our previous direct determination. The amplitudes of the deviations in the DOS depend on the magnetic field via the spatially averaged superconducting order parameter which has a square-root dependence on the magnetic field. Finally, the second Ginzburg-Landau parameter kappa2(T) has been determined from the experimental data., Comment: 11 pages, 5 figures