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BaFe$_2$S$_3$ is a quasi-one-dimensional antiferromagnetic insulator that becomes superconducting under hydrostatic pressure. The magnetic ordering temperature, $T_N$, as well as the presence of superconductivity have been found to be sample dependent. It has been argued that the Fe content may play a decisive role, with the use of 5%mol excess Fe being reportedly required during the synthesis to optimize the magnetic ordering temperature and the superconducting properties. However, it is yet unclear whether an Fe off-stoichiometry is actually present in the samples, and how it affects the structural, magnetic and transport properties. Here, we present a systematic study of compositional, structural and physical properties of BaFe$_{2+��}$S$_3$ as a function of the nominal Fe excess $��$. As $��$ increases, we observe the presence of an increasing fraction of secondary phases but no systematic change in the composition or crystal structure of the main phase. Magnetic susceptibility curves are influenced by the presence of magnetic secondary phases. The previously reported maximum of $T_N$ at $��$=0.1 was not confirmed. Samples with nominal $��$=0 present the lowest $T_N$ and the resistivity anomaly at the highest temperature $T^*$ while, for $��\geq 0.05$, both quantities and the transport gap are seemingly $��$-independent. Finally, we show that crystals free of ferromagnetic spurious phases can be obtained by remelting samples with nominal $��$=0.05 in a Bridgman process., 11 pages, 8 figures

In Eu2ZnIrO6, effectively two atoms are active i.e. Ir is magnetically active, which results in complex magnetic ordering within the Ir sublattice at low temperature. On the other hand, although Eu is a van-vleck paramagnet, it is active in the electronic channels involving 4f 6 crystal-field split levels. Phonons, quanta of lattice vibration, involving vibration of atoms in the unit cell, are intimately coupled with both magnetic and electronic degrees of freedom (DoF). Here, we report a comprehensive study focusing on the phonons as well as intra-configurational excitations in double-perovskite Eu2ZnIrO6. Our studies reveal strong coupling of phonons with the underlying magnetic DoF reflected in the renormalization of the phonon self-energy parameters well above the spin-solid phase (TN ~ 12 K) till temperature as high as ~ 3TN, evidences broken spin rotational symmetry deep into the paramagnetic phase. In particular, all the observed first-order phonon modes show softening of varying degree below ~3TN, and low-frequency phonons become sharper, while the high-frequency phonons show broadening attributed to the additional available magnetic damping channels. We also observed a large number of high-energy modes, 39 in total, attributed to the electronic transitions between 4f-levels of the rare-earth Eu3+ ion and these modes shows anomalous temperature evolution as well as mixing of the crystal-field split levels attributed to the strong coupling of electronic and lattice DoF., 7 figures

We report comprehensive Raman-scattering measurements on a single crystal of double-perovskite Nd2ZnIrO6 in temperature range of 4-330 K, and spanning a broad spectral range from 20 cm-1 to 5500 cm-1. The paper focuses on lattice vibrations and electronic transitions involving Kramers doublets of the rare-earth Nd3+ ion with local C1 site symmetry. Temperature evolution of these quasi-particle excitations have allowed us to ascertain the intricate coupling between lattice and electronic degrees of freedom in Nd2ZnIrO6. Strong coupling between phonons and crystal-field excitation is observed via renormalization of the self-energy parameter of the phonons i.e. peak frequency and line-width. The phonon frequency shows abrupt hardening and line-width narrowing below ~ 100 K for the majority of the observed first-order phonons. We observed splitting of the lowest Kramers doublets of ground state (4I9/2) multiplets i.e. lifting of the Kramers degeneracy, prominently at low-temperature (below ~ 100 K), attributed to the Nd-Nd/Ir exchange interactions and the intricate coupling with the lattice degrees of freedom. The observed splitting is of the order of ~ 2-3 meV and is consistent with the estimated value. We also observed a large number of high-energy modes, 46 in total, attributed to the intra-configurational transitions between 4f3 levels of Nd3+ coupled to the phonons reflected in their anomalous temperature evolution.

The synthesis and characterization of the previously unknown material LaCaScIrO$_6$ is reported. LaCaScIrO$_6$ presents a new example of the rare case of a double perovskite with the strongly spin-orbit coupled 5\textit{d}-ion Ir$^{4+}$ as its only magnetic species, forming a monoclinically distorted version of the frustrated fcc lattice. Magnetization measurements show a weak anomaly at 8~K. The Curie-Weiss temperature \Theta$_{CW}$ and effective magnetic moment \mu$_{eff}$ of LaCaScIrO$_6$ are in close proximity to the related compound La$_2$MgIrO$_6$ but differ from La$_2$ZnIrO$_6$. This suggests that the nature of the non-magnetic \textit{B}-ion, namely its \textit{d}-orbital filling has a strong influence on the magnetic properties. The \textit{d}$^{0}$-ions Sc$^{3+}$ and Mg$^{2+}$ allow a different kind of exchange interactions within the Ir-sublattice than the \textit{d}$^{10}$-ion Zn$^{2+}$. In addition, ac-susceptibility data does not show signs of a spin-glass ground state. The nature of the magnetism in LaCaScIrO$_6$ has been further elucidated using muon spin relaxation measurements. The zero-field measurements reveal the absence of well defined oscillations down to 1.6\,K, while temperature dependent $\mu$SR studies show an anomaly at 8\,K. Overall, our results suggest the presence of two different magnetic environments or domains in LaCaScIrO$_6$, which is likely related to its structural features.

The behavior of spin propagation in metals in various measurement schemes is shown to be qualitatively different than a simple exponential decay - due to the backflow effect on spin diffusion in the presence of interfaces. To probe this effect we utilize the spin sensitivity of an Andreev contact between gold films of variable thickness deposited on top of a spin injector, Co$_{2}$Mn$_{0.5}$Fe$_{0.5}$Si, with the spin polarization of approximately 45\%, and Nb superconducting tip. While the results are consistent with gradually decaying spin polarization as the film thickness increases, the spin diffusion length in Au found to be 285 nm, is more than two times larger that one would have obtained without taking the backflow effect into account.

We report an experimental study of the static magnetization $M(H,T)$ and high-field electron spin resonance (ESR) of polycrystalline \MgGd, a representative member of the newly discovered class of the so-called tripod-kagome antiferromagnets where the isotropic Gd$^{3+}$ spins ($S = 7/2$) form a two-dimensional kagome spin-frustrated lattice. It follows from the analysis of the low-$T$ $M(H)$-curves that the Gd$^{3+}$ spins are coupled by a small isotropic antiferromagnetic (AFM) exchange interaction $|J| \approx$ 0.3\,K. The $M(H,T)$-dependences measured down to 0.5\,K evidence a long-range AFM order at $T_{\text{N}} = 1.7$\,K and its rapid suppression at higher fields $\geq 4$\,T. ESR spectra measured in fields up to 15\,T are analyzed considering possible effects of demagnetizing fields, single-ion anisotropy and spin-spin correlations. While the demagnetization effects due to a large sample magnetization in high fields and its shape anisotropy become relevant at low temperatures, the broadening of the ESR line commencing already at $T\lesssim 30$\,K may indicate the onset of the spin-spin correlations far above the ordering temperature due to the geometrical spin frustration in this compound., Comment: 14 pages, 13 figures, 5 formulas

In this work, we report on the synthesis and magnetic properties of a series of double perovskites Ln$_2$ZnIrO$_6$ with Ln = Nd, Sm, Eu & Gd. These compounds present new examples of the rare case of double perovskites (general formula A$_2$BB'O$_6$) with a magnetic 4f -ion on the A-site in combination with the strongly spin-orbit coupled 5d-transition metal ion Ir$^{4+}$ on the B-sublattice. We discuss the impact of different rare earths on the macroscopic magnetic properties. Gd$_2$ZnIrO$_6$ and Eu$_2$ZnIrO$_6$ show weak canted antiferromagnetic order below T$_N$ = 23 K and T$_N$ = 12 K, respectively. Sm$_2$ZnIrO$_6$ orders antiferromagnetically at T$_N$ = 13 K. Nd$_2$ZnIrO$_6$ exhibits complex magnetic properties with strong field dependence ranging from a two-step behavior at H = 0.01 T to an antiferromagnetic ground state at intermediate external fields and a spin-flop phase at H$\geq$4 T, which suggests complex interplay between Nd$^{3+}$ and Ir$^{4+}$ . To further shed light on this magnetic interaction, the magnetic structure of Nd$_2$ZnIrO$_6$'s ground state is examined via neutron powder diffraction.

The quest for Kitaev spin liquids in particular three dimensional solids is long sought goal in condensed matter physics, as these states may give rise to exotic new types of quasi-particle excitations carrying fractional quantum numbers namely Majorana Fermionic excitations. Here we report the experimental signature of this characteristic feature of the Kitaev spin liquid via Raman measurements. Sm2ZnIrO6 is a strongly spin orbit coupled Mott insulator, where Jeff = 1/2 controls the physics, which provide striking evidence for this characteristic feature of the Kitaev spin liquid. As the temperature is lowered, we find that the spin excitations form a continuum in contrast to the conventional sharp modes expected in ordered antiferromagnets. Our observation of a broad magnetic continuum and anomalous renormalization of the phonon self-energy parameters evidence the existence of Majorana fermions from spin fractionalization in double perovskites structure as theoretically conjectured in a Kitaev-Heisenberg geometrically frustrated double perovskite systems.

We report electron spin resonance (ESR) spectroscopy results on the double perovskite Ba$_2$YIrO$_6$. On general grounds, this material is expected to be nonmagnetic due to the strong coupling of the spin and orbital momenta of Ir$^{5+}$ (5$d^4$) ions. However, controversial experimental reports on either strong antiferromagnetism with static order at low temperatures or just a weakly paramagnetic behavior have triggered a discussion on the breakdown of the generally accepted scenario of the strongly spin-orbit coupled ground states in the 5$d^4$ iridates and the emergence of a novel exotic magnetic state. Our data evidence that the magnetism of the studied material is solely due to a few percent of Ir$^{4+}$ and Ir$^{6+}$ magnetic defects while the regular Ir$^{5+}$ sites remain nonmagnetic. Remarkably, the defect Ir$^{6+}$ species manifest magnetic correlations in the ESR spectra at $T\lesssim 20$ K suggesting a long-range character of superexchange in the double prevoskites as proposed by recent theories.

We report $^{75}$As nuclear magnetic resonance measurements on single crystals of RbFe$_{2}$As$_{2}$ and CsFe$_{2}$As$_{2}$. Taking previously reported results for KFe$_{2}$As$_{2}$ into account, we find that the anisotropic electronic correlations evolve towards a magnetic instability in the $A$Fe$_{2}$As$_{2}$ series (with $A$ = K, Rb, Cs). Upon isovalent substitution with larger alkali ions, a drastic enhancement of the anisotropic nuclear spin-lattice relaxation rate and decreasing Knight shift reveal the formation of pronounced spin fluctuations with stripe-type modulation. Furthermore, a decreasing power-law exponent of the nuclear spin-lattice relaxation rate $(1/T_{1})_{H\parallel{ab}}$, probing the in-plane spin fluctuations, evidences an emergent deviation from Fermi-liquid behavior. All these findings clearly indicate that the expansion of the lattice in the $A$Fe$_{2}$As$_{2}$ series tunes the electronic correlations towards a quantum critical point at the transition to a yet unobserved, ordered phase., 5 pages, 4 figures

We present a microscopic investigation of frequently observed impurity-induced states in stoichiometric LiFeAs using low temperature scanning tunneling microscopy and spectroscopy (STM/STS). Our data reveal seven distinct well defined defects which are discernible in topographic measurements. Depending on their local topographic symmetry, we are able to assign five defect types to specific lattice sites at the Li, Fe and As positions. The most prominent result is that two different defect types have a remarkably different impact on the superconducting state. A specific and quite abundant Fe-defect with $D_2$-symmetry generates significant impurity-induced additional states primarily at positive bias voltage with pronounced peaks in the on-site local density of states (LDOS) at about 4~mV and 12~mV. On the other hand, a $D_4$-symmetric As-defect causes a significantly enhanced LDOS at both positive and negative bias voltages. We expect that these findings provide fresh input for further experimental and theoretical studies on elucidating the nature of superconductivity in LiFeAs.

We report the structural, magnetic and thermodynamic properties of the double perovskite compound La2CuIrO6 from X-ray, neutron diffraction, neutron depolarization, dc magnetization, ac susceptibility, specific heat, muon-spin-relaxation (uSR), electron-spin-resonance (ESR) and nuclear magnetic resonance (NMR) measurements. Below ~113 K, short-range spin-spin correlations occur within the Cu2+ sublattice. With decreasing temperature, the Ir4+ sublattice progressively involves in the correlation process. Below T = 74 K, the magnetic sublattices of Cu (spin s = 1/2) and Ir (pseudospin j = 1/2) in La2CuIrO6 are strongly coupled and exhibit an antiferromagnetic phase transition into a non-collinear magnetic structure accompanied by a small uncompensated transverse moment. A weak anomaly in ac-susceptibility as well as in the NMR and {\mu}SR spin lattice relaxation rates at 54 K is interpreted as a cooperative ordering of the transverse moments which is influenced by the strong spin-orbit coupled 5d ion Ir4+. We argue that the rich magnetic behaviour observed in La2CuIrO6 is related to complex magnetic interactions between the strongly correlated spin-only 3d ions with the strongly spin-orbit coupled 5d transition ions where a combination of the spin-orbit coupling and the low-symmetry of the crystal lattice plays a special role for the spin structure in the magnetically ordered state., Comment: 15 Pages, 18 figures, To appear in PRB

In this article we review our angle- and time-resolved photoemission studies (ARPES and trARPES) on various ferropnictides.

Recently, the iridate double perovskite Sr$_2$YIrO$_6$ has attracted considerable attention due to the report of unexpected magnetism in this Ir$^{5+}$ (5d$^4$) material, in which according to the J$_{eff}$ model, a non-magnetic ground state is expected. However, in recent works on polycrystalline samples of the series Ba$_{2-x}$Sr$_x$YIrO$_6$ no indication of magnetic transitions have been found. We present a structural, magnetic and thermodynamic characterization of Sr$_2$YIrO$_6$ single crystals, with emphasis on the temperature and magnetic field dependence of the specific heat. Here, we demonstrate the clue role of single crystal X-ray diffraction on the structural characterization of the Sr$_2$YIrO$_6$ double perovskite crystals by reporting the detection of a $\sqrt{2}a \times \sqrt{2}a \times 1c$ supercell, where $a$, $b$ and $c$ are the unit cell dimensions of the reported monoclinic subcell. In agreement with the expected non-magnetic ground state of Ir$^{5+}$ (5d$^4$) in Sr$_2$YIrO$_6$, no magnetic transition is observed down to 430~mK. Moreover, our results suggest that the low temperature anomaly observed in the specific heat is not related to the onset of long-range magnetic order. Instead, it is identified as a Schottky anomaly caused by paramagnetic impurities present in the sample, of the order of $n \sim 0.5(2)$ \%. These impurities lead to non-negligible spin correlations, which nonetheless, are not associated with long-range magnetic ordering., 20 pages, 10 figures

We report on measurements of the sound velocity and attenuation in a single crystal of the candidate quantum- spin-ice material Yb$_2$Ti$_2$O$_7$ as a function of temperature and magnetic field. The acoustic modes couple to the spins magneto-elastically and, hence, carry information about the spin correlations that sheds light on the intricate magnetic phase diagram of Yb$_2$Ti$_2$O$_7$ and the nature of spin dynamics in the material. Particularly, we find a pronounced thermal hysteresis in the acoustic data with a concomitant peak in the specific heat indicating a possible first-order phase transition at about $0.17$ K. At low temperatures, the acoustic response to magnetic field saturates hinting at the development of magnetic order. Furthermore, mean-field calculations suggest that Yb$_2$Ti$_2$O$_7$ undergoes a first-order phase transition from a cooperative paramagnetic phase to a ferromagnet below $T\approx 0.17$ K., Comment: 8 pages

The deliberate insertion of magnetic Mn dopants in the Fe sites of the optimally-doped SmFeAsO0.88-F0.12 iron-based superconductor can modify in a controlled way its electronic properties. The resulting phase diagram was investigated across a wide range of manganese contents (x) by means of muon-spin spectroscopy (muSR), both in zero- and in transverse fields, respectively, to probe the magnetic and the superconducting order. The pure superconducting phase (at x < 0.03) is replaced by a crossover region at intermediate Mn values (0.03 =< x < 0.08), where superconductivity coexists with static magnetic order. After completely suppressing superconductivity for x = 0.08, a further increase in Mn content reinforces the natural tendency towards antiferromagnetic correlations among the magnetic Mn ions. The sharp drop of Tc and the induced magnetic order in the presence of magnetic disorder/dopants, such as Mn, are both consistent with a recent theoretical model of unconventional superconductors [M. Gastiasoro et al., ArXiv 1606.09495], which includes correlation-enhanced RKKY-couplings between the impurity moments., 10 pages, 13 figures. Accepted on Physical Review B

Modern theories of quantum magnetism predict exotic multipolar states in weakly interacting strongly frustrated spin-1/2 Heisenberg chains with ferromagnetic nearest neighbor (NN) inchain exchange in high magnetic fields. Experimentally these states remained elusive so far. Here we report the evidence for a long-sought magnetic field-induced nematic state arising above a field of $\sim 13$ T in the edge-sharing chain cuprate LiSbCuO$_4$ $\equiv$ LiCuSbO$_4$. This interpretation is based on the observation of a field induced spin-gap in the measurements of the $^7$Li NMR spin relaxation rate $T_1^{-1}$ as well as a contrasting field-dependent power-law behavior of $T_1^{-1}$ vs. $T$ and is further supported by static magnetization and ESR data. An underlying theoretical microscopic approach favoring a nematic scenario is based essentially on the NN XYZ exchange anisotropy within a model for frustrated spin-1/2 chains. It is investigated by the DMRG technique. The employed exchange parameters are justified qualitatively by electronic structure calculations for LiCuSbO$_4$.

Materials with a 5d4 electronic configuration are generally considered to have a nonmagnetic ground state (J=0). Interestingly, Sr2YIrO6 (Ir5+ having 5d4 electronic configuration) was recently reported to exhibit long-range magnetic order at low temperature and the distorted IrO6 octahedra were discussed to cause the magnetism in this material. Hence, a comparison of structurally distorted Sr2YIrO6 with cubic Ba2YIrO6 may shed light on the source of magnetism in such Ir5+ materials with 5d4 configuration. Besides, Ir5+ materials having 5d4 are also interesting in the context of recently predicted excitonic types of magnetism. Here we report a single-crystal-based analysis of the structural, magnetic, and thermodynamic properties of Ba2YIrO6. We observe that in Ba2YIrO6 for temperatures down to 0.4 K, long-range magnetic order is absent but at the same time correlated magnetic moments are present. We show that these moments are absent in fully relativistic ab initio band-structure calculations; hence, their origin is presently unclear., Comment: 8 pages, 9 figures

Muon Spin Rotation ($\mu$SR) and $^{19}$F Nuclear Magnetic Resonance (NMR) measurements were performed to investigate the effect of Mn for Fe substitutions in La$_{1-y}$Y$_{y}$Fe$_{1-x}$Mn$_x$AsO$_{0.89}$F$_{0.11}$ superconductors. While for $y = 0$ a very low critical concentration of Mn ($x = 0.2$%) is needed to quench superconductivity, as $y$ increases the negative chemical pressure introduced by Y for La substitution stabilizes superconductivity and for $y= 20$% it is suppressed at Mn contents an order of magnitude larger. A magnetic phase arises once superconductivity is suppressed both for $y$=0 and for $y= 20$%. Low-energy spin fluctuations give rise to a peak in $^{19}$F NMR $1/T_1$ with an onset well above the superconducting transition temperature and whose magnitude increases with $x$. Also the static magnetic correlations probed by $^{19}$F NMR linewidth measurements show a marked increase with Mn content. The disruption of superconductivity and the onset of the magnetic ground-state are discussed in the light of the proximity of LaFeAsO$_{0.89}$F$_{0.11}$ to a quantum critical point., Comment: 8 pages, 9 figures

We have performed temperature dependent tunneling spectroscopy on an impurity-free surface area of a LiFeAs single crystal. Our data reveal a highly unusual temperature evolution of superconductivity: at $T_c^*=18$~K a partial superconducting gap opens, as is evidenced by subtle, yet clear features in the tunneling spectra, i.e. particle-hole symmetric coherence peaks, and a dip-hump structure which signals strong-coupling superconductivity. At $T_c=16$~K, these features substantiate dramatically and become characteristic of full superconductivity. Remarkably, this is accompanied by an almost jump-like increase of the gap energy at $T_c$ to about 87\% of its low-temperature gap value. The energy of the bosonic mode as measured by the distance between the coherence peak and the higher-energy dip remains practically constant in the whole temperature regime $T\leq T_c^*$. The comparison of these findings with established experimental and theoretical results lead us to suggest that the bosonic mode is not directly related to incommensurate spin fluctuations that have previously been observed in inelastic neutron scattering., 6 pages, 4 figures

A 63Cu NMR study of Pb-doped Bi:2201 system, Bi1.6Pb0.4Sr2.05CuOy, is presented. Temperature dependencies of the NMR peak shift and the nuclear spin-lattice relaxation rate revealed the pseudogap that opens at T* = 20 - 60 K, way above the Tc ~ 9K measured for the orientation (H//c) and value (7 T) of the NMR experiment field. The noticeable discrepancy between Tc and T* and the behavior of Cu SLR at T > T* imply the underdoped state of the studied system. The magnetic field has a relatively weak effect on the superconductivity in the studied system, as evidenced from small (7-8 K) shift of the zero-field Tc = 16+/- 1K under the applied 7 T field. This fact suggests a high value of the upper critical field, unusual for a compound with such low Tc., 4 pages, 4 figures

$^{19}$F NMR measurements in optimally electron-doped La$_{1-y}$Y$_{y}$Fe$_{1-x}$Mn$_{x}$AsO$_{0.89}$F$_{0.11}$ superconductors are presented. In these materials the effect of Mn doping on the superconducting phase is studied for two series of compounds ($y= 0$ and $y= 0.2$) where the chemical pressure is varied by substituting La with Y. In the $y=0.2$ series superconductivity is suppressed for Mn contents an order of magnitude larger than for the $y=0$ series. For both series a peak in the $^{19}$F NMR nuclear spin-lattice relaxation rate $1/T_1$ emerges upon Mn doping and gets significantly enhanced on approaching the quantum phase transition between the superconducting and magnetic phases. $^{19}$F NMR linewidth measurements show that for similar Mn contents magnetic correlations are more pronounced in the $y=0$ series, at variance with what one would expect for $\vec Q=(\pi/a,0)$ spin correlations. These observations suggest that Mn doping tends to reduce fluctuations at $\vec Q=(\pi/a,0)$ and to enhance other low-frequency modes. The effect of this transfer of spectral weight on the superconducting pairing is discussed along with the charge localization induced by Mn., Comment: 5 pages, 5 figures

Strong electron interactions in solids increase effective mass, and shrink the electronic bands [1]. One of the most unique and robust experimental facts about iron-based superconductors [2-4] is the renormalization of the conduction band by factor of 3 near the Fermi level [5-9]. Obviously related to superconductivity, this unusual behaviour remains unexplained. Here, by studying the momentum-resolved spectrum of the whole valence band in a representative material, we show that this phenomenon originates from electronic interaction on a much larger energy scale. We observe an abrupt depletion of the spectral weight in the middle of the Fe $3d$ band, which is accompanied by a drastic increase of the scattering rate. Remarkably, all spectral anomalies including the low-energy renormalization can be explained by coupling to excitations, strongly peaked at about 0.5 eV. Such high-energy interaction distinguishes all unconventional superconductors from common metals.

We report an experimental and theoretical investigation of the electron-boson interaction in KFe2As2 by point-contact (PC) spectroscopy, model, and ab-initio LDA-based calculations for the standard electron-phonon Eliashberg function. The PC spectrum viz. the second derivative of the I - V characteristic of representative PC exhibits a pronounced maximum at about 20meV and surprisingly a featureless behavior at lower and higher energies. We discuss phonon and non-phonon (excitonic) mechanisms for the origin of this peak. Analysis of the underlying source of this peak may be important for the understanding of serious puzzles of superconductivity in this type of compounds., 10 pages, 6 figs., to be published in PRB

We present an inelastic neutron scattering study on single-crystalline LiFeAs devoted to the characterization of the incommensurate antiferromagnetic fluctuations at $\mathbf{Q}=(0.5\pm\delta, 0.5\mp\delta, q_l)$. Time-of-flight measurements show the presence of these magnetic fluctuations up to an energy transfer of 60 meV, while polarized neutrons in combination with longitudinal polarization analysis on a triple-axis spectrometer prove the pure magnetic origin of this signal. The normalization of the magnetic scattering to an absolute scale yields that magnetic fluctuations in LiFeAs are by a factor eight weaker than the resonance signal in nearly optimally Co-doped BaFe$_2$As$_2$, although a factor two is recovered due to the split peaks owing to the incommensurability. The longitudinal polarization analysis indicates weak spin space anisotropy with slightly stronger out-of-plane component between 6 and 12 meV. Furthermore, our data suggest a fine structure of the magnetic signal most likely arising from superposing nesting vectors., Comment: 9 pages, 8 figures

A commercially available calorimeter has been used to investigate the specific heat of a high-quality \kn\ single crystal. The addenda heat capacity of the calorimeter is determined in the temperature range $0.02 \, \mathrm{K} \leq T \leq 0.54 \, \mathrm{K}$. The data of the \kn\ crystal imply the presence of a large $T^2$ contribution to the specific heat which gives evidence of $d$-wave order parameter symmetry in the superconducting state. To improve the measurements, a novel design for a calorimeter with a paramagnetic temperature sensor is presented. It promises a temperature resolution of $\Delta T \approx 0.1 \, \mathrm{\mu K}$ and an addenda heat capacity less than $200 \, \mathrm{pJ/K}$ at $ T < 100 \, \mathrm{mK}$., Comment: 8 pages, 5 figures

We have studied the magnetic ordering in Na doped BaFe$_2$As$_2$ by unpolarized and polarized neutron diffraction using single crystals. Unlike previously studied FeAs-based compounds that magnetically order, Ba$_{1-x}$Na$_x$Fe$_2$As$_2$ exhibits two successive magnetic transitions: For x=0.35 upon cooling magnetic order occurs at $\sim$70\ K with in-plane magnetic moments being arranged as in pure or Ni, Co and K-doped BaFe$_2$As$_2$ samples. At a temperature of $\sim$46\ K a second phase transition occurs, which the single-crystal neutron diffraction experiments can unambiguously identify as a spin reorientation. At low temperatures, the ordered magnetic moments in Ba$_{0.65}$Na$_{0.35}$Fe$_2$As$_2$ point along the $c$ direction. Magnetic correlations in these materials cannot be considered as Ising like, and spin-orbit coupling must be included in a quantitative theory., Comment: 5 pages, 4 figures

We present study of derivatives of current-voltage I(V) characteristics of point-contacts (PCs) based on Ba{1-x}Na{x}Fe2As2 (x=0.25) in the normal and superconducting state. The detailed analysis of dV/dI(V) data (also given in Appendix A) shows that the thermal regime, when temperature increases with a voltage at a rate of about 1.8 K/mV, is realized in the investigated PCs at least at high biases V above the superconducting (SC) gap \Delta. In this case, specific resistivity \rho (T) in PC core is responsible for a peculiar dV/dI(V) behavior, while a pronounced asymmetry of dV/dI(V) is caused by large value of thermopower in this material. A reproducible zero-bias minima detected on dV/dI(V) at low biases in the range \pm(6--9)mV well below the SC critical temperature T_c could be connected with the manifestation of the SC gap \Delta. Evaluation of these Andreev-reflection-like structures on dV/dI(V) points out to the preferred value of 2\Delta/kT_c \approx 6. The expected second gap features on dV/dI(V) are hard to resolve unambiguously, likely due to impurity scattering, spatial inhomogeneity and transition to the mentioned thermal regime as the bias further increases. Suggestions are made how to separate spectroscopic features in dV/dI(V) from those caused by the thermal regime., Comment: 10 pages, 15 figs, two Apps, to be published in PRB

We present a detailed local probe study of the magnetic order in the oxychalcogenide La2O2Fe2OSe2 utilizing 57Fe Moessbauer, 139La NMR, and muon spin relaxation spectroscopy. This system can be regarded as an insulating reference system of the Fe arsenide and chalcogenide superconductors. From the combination of the local probe techniques we identify a non-collinear magnetic structure similar to Sr2F2Fe2OS2. The analysis of the magnetic order parameter yields an ordering temperature TN = 90.1 K and a critical exponent of beta = 0.133, which is close to the 2D Ising universality class as reported in the related oxychalcogenide family.

The effect of hydrostatic pressure and partial Na substitution on the normal-state properties and the superconducting transition temperature ($T_c$) of K$_{1-x}$Na$_x$Fe$_2$As$_2$ single crystals were investigated. It was found that a partial Na substitution leads to a deviation from the standard $T^2$ Fermi-liquid behavior in the temperature dependence of the normal-state resistivity. It was demonstrated that non-Fermi liquid like behavior of the resistivity for K$_{1-x}$Na$_{x}$Fe$_2$As$_2$ and some KFe$_2$As$_2$ samples can be explained by disorder effect in the multiband system with rather different quasiparticle effective masses. Concerning the superconducting state our data support the presence of a shallow minimum around 2 GPa in the pressure dependence of $T_c$ for stoichiometric KFe$_2$As$_2$. The analysis of $T_c$ in the K$_{1-x}$Na$_{x}$Fe$_2$As$_2$ at pressures below 1.5 GPa showed, that the reduction of $T_c$ with Na substitution follows the Abrikosov-Gor'kov law with the critical temperature $T_{c0}$ of the clean system (without pair-breaking) which linearly depends on the pressure. Our observations, also, suggest that $T_c$ of K$_{1-x}$Na$_x$Fe$_2$As$_2$ is nearly independent of the lattice compression produced by the Na substitution. Further, we theoretically analyzed the behavior of the band structure under pressure within the generalized gradient approximation (GGA). A qualitative agreement between the calculated and the recently in de Haas-van Alphen experiments [T. Terashima et al., Phys.Rev.B89, 134520(2014)] measured pressure dependencies of the Fermi-surface cross-sections has been found. These calculations, also, indicate that the observed minimum around 2~GPa in the pressure dependence of $T_c$ may occur without a change of the pairing symmetry.

We present femtosecond time-resolved pump-probe spectroscopic studies of a pseudogap (PG) along with the superconducting (SC) gap in an overdoped iron pnictide Ca(Fe0.927Co0.073)2As2. It is seen that the temperature evolution of the photoexcited quasiparticle (QP) relaxation dynamics, coherently excited A1g-symmetric optical phonon and two acoustic phonon dynamics behave anomalously in the vicinity of the superconducting transition temperature Tc. A continuous change in the sign of the experimentally measured transient differential reflectivity Delta_R/R signal at the zero time-delay between the pump and probe pulses at a temperature of ~200 K is inferred as an evidence of the emergence of the PG phase around that temperature. This behavior is independent of the pump photon energy and occurs for crystals without the spin density wave phase transition., Comment: EPL (2014)

We present a detailed experimental study of bulk and powder samples of the Heusler shape memory alloy Ni$_2$MnGa, including zero-field static and dynamic $^{55}$Mn NMR experiments, X-ray powder diffraction and magnetization experiments. The NMR spectra give direct access to the sequence of structural phase transitions in this compound, from the high-T austenitic phase down to the low-T martensitic phase. In addition, a detailed investigation of the so-called rf-enhancement factor provides local information for the magnetic stiffness and restoring fields for each separate coordination, structural, crystallographic environment, thus differentiating signals coming from austenitic and martensitic components. The temperature evolution of the NMR spectra and the rf-enhancement factors shows strong dependence on sample preparation. In particular, we find that sample powderization gives rise to a significant portion of martensitic traces inside the high-T austenitic region, and that these traces can be subsequently removed by annealing.

We report a low-temperature specific heat study of high-quality single crystals of the heavily hole doped superconductor Ca$_{0.32}$Na$_{0.68}$Fe$_2$As$_2$. This compound exhibits bulk superconductivity with a transition temperature $T_c \approx 34$\,K, which is evident from the magnetization, transport, and specific heat measurements. The zero field data manifests a significant electronic specific heat in the normal state with a Sommerfeld coefficient $\gamma \approx 53$ mJ/mol K$^{2}$. Using a multi-band Eliashberg analysis, we demonstrate that the dependence of the zero field specific heat in the superconducting state is well described by a three-band model with an unconventional s$_\pm$ pairing symmetry and gap magnitudes $\Delta_i$ of approximately 2.35, 7.48, and -7.50 meV. Our analysis indicates a non-negligible attractive intraband coupling,which contributes significantly to the relatively high value of $T_c$. The Fermi surface averaged repulsive and attractive coupling strengths are of comparable size and outside the strong coupling limit frequently adopted for describing high-$T_c$ iron pnictide superconductors. We further infer a total mass renormalization of the order of five, including the effects of correlations and electron-boson interactions., Comment: 8 Figures, Submitted to PRB

We present a systematic study of the electronic specific heat jump ($��C_{\rm el}$) at the superconducting transition temperature $T_c$ of K$_{1-x}$Na$_x$Fe$_2$As$_2$. Both $T_c$ and $��C_{\rm el}$ monotonously decrease with increasing $x$. The specific heat jump scales approximately with a power-law, $��C_{\rm el} \propto T_c^��$, with $��\approx 2$ determined by the impurity scattering rate, in contrast to most iron-pnictide superconductors, where the remarkable Bud'ko-Ni-Canfield (BNC) scaling $��C_{\rm el} \propto T^3$ has been found. Both the $T$ dependence of $C_{\rm el}(T)$ in the superconducting state and the nearly quadratic scaling of $��C_{\rm el}$ at $T_c$ are well described by the Eliashberg-theory for a two-band $d$-wave superconductor with weak pair-breaking due to nonmagnetic impurities. The disorder induced by the Na substitution significantly suppresses the small gaps leading to gapless states in the slightly disordered superconductor, which results in a large observed residual Sommerfeld coefficient in the superconducting state for $x > 0$., 5 pages, 3 figures, and supplement

Type, degree and evolution of structural order are important aspects for understanding and controlling the properties of highly spin polarized Heusler compounds, in particular with respect to the optimal film growth procedure. In this work, we compare the structural order and the local magnetic properties revealed by nuclear magnetic resonance (NMR) spectroscopy with the macroscopic properties of thin Co$_2$FeAl$_{0.5}$Si$_{0.5}$ Heusler films with varying thickness. A detailed analysis of the measured NMR spectra presented in this paper enables us to find a very high degree of $L2_1$ type ordering up to 81% concomitantly with excess Fe of 8 to 13% at the expense of Al and Si. We show, that the formation of certain types of order do not only depend on the thermodynamic phase diagrams as in bulk samples, but that the kinetic control may contribute to the phase formation in thin films. It is an exciting finding that Co$_2$FeAl$_{0.5}$Si$_{0.5}$ can form an almost ideal $L2_1$ structure in films though with a considerable amount of Fe-Al/Si off-stoichiometry. Moreover, the very good quality of the films as demonstrated by our NMR study suggests that the novel technique of off-axis sputtering technique used to grow the films sets stage for the optimized performance of Co$_2$FeAl$_{0.5}$Si$_{0.5}$ in spintronic devices., Published in Phys. Rev. B

From the measurement and analysis of the specific heat of high-quality K_(1-x)Na_xFe_2As_2 single crystals we establish the presence of large T^2 contributions with coefficients alpha_sc ~ 30 mJ/mol K^3 at low-T for both x=0 and 0.1. Together with the observed square root field behavior of the specific heat in the superconducting state both findings evidence d-wave superconductivity on almost all Fermi surface sheets with an average gap amplitude of Delta_0 in the range of 0.4 - 0.8 meV. The derived Delta_0 and the observed T_c agree well with the values calculated within the Eliashberg theory, adopting a spin-fluctuation mediated pairing in the intermediate coupling regime., Comment: 8 pages, 5 figures, field dependence of the specific heat added, slightly changed title, changed sequence of authors, one author added, accepted by Phys. Rev. B Rapid Communications

We provide direct experimental evidence for the identical effect of the in-plane Fe$_{1-x}$Co$_{x}$ and of the out-of-plane O$_{1-x}$F$_{x}$ chemical dilutions on the itinerant spin-density-wave (SDW) magnetic phase in CeFeAsO. Remarkably, the suppression of SDW is not sensitive at all to the different kinds of disorder introduced in the two cases. Still, it is clearly shown that the sizeable in-plane disorder induced by the Fe$_{1-x}$Co$_{x}$ substitution is highly effective in suppressing $T_{\textrm{c}}$. Differently from what is observed in CeFeAsO$_{1-x}$F$_{x}$, the ordered magnetic phase of the Ce sublattice is preserved throughout the whole phase diagram in CeFe$_{1-x}$Co$_{x}$AsO ($x \leq 0.2$). An intriguing effect is encountered, whereby the magnetic coupling among Ce$^{3+}$ ions is enhanced by the superconducting phase., Comment: 8 pages (Main text: 4 pages. Paper merged with supplemental information)

We report a systematic study on the electronic structure and superconducting (SC) gaps in electron doped NaFe$_{0.95}$Co$_{0.05}$As superconductor using angle-resolved photoemission spectroscopy. Hole-like Fermi sheets are at the zone center and electron-like Fermi sheets are at the zone corner, and are mainly contributed by $xz$ and $yz$ orbital characters. Our results reveal a $\frac{\Delta}{K_B T_c}$ in the range of 1.8-2.1, suggesting a weak-coupling superconductivity in these compounds. Gap closing above the transition temperature ($T_c$) shows the absence of pseudogaps. Gap evolution with temperature follow the BCS gap equation near the $\Gamma$, $Z$, and $M$ high symmetry points. Furthermore, an almost isotropic superconductivity along $k_z$ direction in the momentum space is observed by varying the excitation energies., Comment: 6 pages, 5 figures, Accepted by Phy.Rev.B

Co2FeSi, a Heusler alloy with the highest magnetic moment per unit cell and the highest Curie temperature, has largely been described theoretically as a half-metal. This conclusion, however, disagrees with Point Contact Andreev Reflection (PCAR) spectroscopy measurements, which give much lower values of spin polarization, P. Here, we present the spin polarization measurements of Co2FeSi by the PCAR technique, along with a thorough computational exploration, within the DFT and a GGA+U approach, of the Coulomb exchange U-parameters for Co and Fe atoms, taking into account spin-orbit coupling. We find that the orbital contribution (mo) to the total magnetic moment (mT) is significant, since it is at least 3 times greater than the experimental uncertainty of mT. Account of mo radically affects the acceptable values of U. Specifically, we find no values of U that would simultaneously satisfy the experimental values of the magnetic moment and result in the half-metallicity of Co2FeSi. On the other hand, the ranges of U that we report as acceptable are compatible with spin polarization measurements (ours and the ones found in the literature), which all are within approximately 40-60% range. Thus, based on reconciling experimental and computational results, we conclude that: a) spin-orbit coupling cannot be neglected in calculating Co2FeSi magnetic properties, and b) Co2FeSi Heusler alloy is not half-metallic. We believe that our approach can be applied to other Heusler alloys such as Co2FeAl., 5 pages, 3 figures

In this work we present the results of the bulk magnetization measurements in a superconducting state of single crystals of Ba$_{0.65}$Na$_{0.35}$Fe$_2$As$_2$. The isothermal magnetic field ($H||c$ axis) dependent magnetization ($M$) loops exhibit a second peak (SP) or `fishtail effect', as well as remarkable flux jumps at low temperatures. The critical current density $J_c$ obtained from the $M(H)$ loops is rather high, of the order of 10$^6$ A/cm$^2$. The analysis of the temperature and field dependent $J_c$ implies that high $J_c$ is mainly due to collective (weak) pinning of vortices by dense microscopic point defects with some contribution from a strong pinning mechanism. Pronounced magnetic instabilities in terms of flux jumps depend strongly on temperature as well on the field sweep rate. The field for first flux jump as calculated from an adiabatic model, however, is much lower than the experimentally observed values, and this enhanced stability is attributed to a flux creep phenomenon. The analysis of field dependent magnetic relaxation data additionally supports a collective pinning model. The data further suggests that SP in M(H) is likely related to crossover in creep dynamics from elastic to plastic mechanism. We have constructed the vortex phase diagram on field-temperature plane., 8 pages, 10 figures

High-quality KFe2As2 single crystals have been studied by transport, magnetization and low-T specific heat measurements. Their analysis shows that superconductivity occurs (in some cases coexists) in the vicinity of disordered magnetic phases (Griffiths and spin-glass type) depending of the amount of local magnetic moments (probably excess Fe derived)and sample inhomogeneity. The achieved phenomenological description of our data including also data from the literature provides a consistent explanation of the observed non-Fermi-liquid behavior and of the nominally large experimental Sommerfeld coefficient gamma_n about 94 mJ/mol K^2. We suggest that the intrinsic value (directly related to the itinerant quasi-particles) gamma_el about 60(10)mJ/mol K^2 is significantly reduced compared with gamma_n. Then an enhanced relative jump of the electronic specific heat Delta C_el/gamma_el T_c about 0.8 and a weak total electron-boson coupling constant lambda less or about 1 follow., 6 pages, 4 figures (including supplement)

Single crystals of Ba$_{1-x}$Na$_x$Fe$_2$As$_2$ with $x$ = 0, 0.25, 0.35, 0.4 were grown using a self-flux high temperature solution growth technique. The superconducting and normal state properties were studied by temperature dependent magnetic susceptibility, electrical resistivity and specific heat revealing that the magnetic and structural transition is rapidly suppressed upon Na-substitution at the Ba-site in BaFe$_2$As$_2$, giving rise to superconductivity. A superconducting transition as high as 34 K is reached for a Na-content of $x$=0.4. The positive Hall coefficient confirms that the substitution of Ba by Na results in hole-doping similarly to the substitution of Ba by K. Angle resolved photoemission spectroscopy was performed on all Ba$_{1-x}$Na$_x$Fe$_2$As$_2$ crystals. The Fermi surface of hole-doped Ba$_{1-x}$Na$_x$Fe$_2$As$_2$ is to high extent the same as the Fermi surface found for the K-doped sister compounds, suggesting a similar impact of the substitution of Ba by either K or Na on the electronic band dispersion at the Fermi level

The anisotropy of the magnetic excitations in BaFe$_2$As$_2$ was studied by polarized inelastic neutron scattering which allows one to separate the components of the magnetic response. Despite the in-plane orientation of the static ordered moment we find the in-plane polarized magnons to exhibit a larger gap than the out-of-plane polarized ones indicating very strong single-ion anisotropy within the layers. It costs more energy to rotate a spin within the orthorhombic {\it a-b} plane than rotating it perpendicular to the FeAs layers., Comment: 4 pages, 4 figures

Electronic structure of newly synthesized single crystals of calcium iron arsenide doped with sodium with Tc ranging from 33 to 14 K has been determined by angle-resolved photoemission spectroscopy (ARPES). The measured band dispersion is in general agreement with theoretical calculations, nonetheless implies absence of Fermi surface nesting at antiferromagnetic vector. A clearly developing below Tc strongly band-dependant superconducting gap has been revealed for samples with various doping levels. BCS ratio for optimal doping, $2\Delta/k_{\rm B}T_{\rm c}=5.5$, is substantially smaller than the numbers reported for related compounds, implying a non-trivial relation between electronic dispersion and superconducting gap in iron arsenides., Comment: first ARPES on CNFA

Among numerous hypotheses, recently proposed to explain superconductivity in iron-based superconductors [1-9], many consider Fermi surface (FS) nesting [2, 4, 8, 10] and dimensionality [4, 9] as important contributors. Precise determination of the electronic spectrum and its modification by superconductivity, crucial for further theoretical advance, were hindered by a rich structure of the FS [11-17]. Here, using the angle-resolved photoemission spectroscopy (ARPES) with resolution of all three components of electron momentum and electronic states symmetry, we disentangle the electronic structure of hole-doped BaFe2As2, and show that nesting and dimensionality of FS sheets have no immediate relation to the superconducting pairing. Alternatively a clear correlation between the orbital character of the electronic states and their propensity to superconductivity is observed: the magnitude of the superconducting gap maximizes at 10.5 meV exclusively for iron 3dxz;yz orbitals, while for others drops to 3.5 meV. Presented results reveal similarities of electronic response to superconducting and magneto-structural transitions [18, 19], implying that relation between these two phases is more intimate than just competition for FS, and demonstrate importance of orbital physics in iron superconductors., Comment: read me

We report ultrafast quasiparticle (QP) dynamics and coherent acoustic phonons in undoped CaFe_2As_2 iron pnictide single crystals exhibiting spin-density wave (SDW) and concurrent structural phase transition at temperature TSDW ~ 165 K using femtosecond time-resolved pump-probe spectroscopy. The contributions in transient differential reflectivity arising from exponentially decaying QP relaxation and oscillatory coherent acoustic phonon mode show large variations in the vicinity of T_SDW. From the temperature-dependence of the QP recombination dynamics in the SDW phase, we evaluate a BCS-like temperature dependent charge gap with its zero-temperature value of ~(1.6+/-0.2)k_BT_SDW, whereas, much above T_SDW, an electron-phonon coupling constant of ~0.13 has been estimated from the linear temperature-dependence of the QP relaxation time. The long-wavelength coherent acoustic phonons with typical time-period of ~100 ps have been analyzed in the light of propagating strain pulse model providing important results for the optical constants, sounds velocity and the elastic modulus of the crystal in the whole temperature range of 3 K to 300 K., Comment: Revised version (to appear as Full Paper in Journal of Physical Society of Japan (2013)); http://jpsj.ipap.jp/link?JPSJ/82/044715/

We report temperature evolution of coherently excited acoustic and optical phonon dynamics in superconducting iron pnictide single crystal Ca(Fe_0.944Co_0.056)_2As_2 across the spin density wave transition at T_SDW ~ 85 K and superconducting transition at T_SC ~20 K. Strain pulse propagation model applied to the generation of the acoustic phonons yields the temperature dependence of the optical constants, and longitudinal and transverse sound velocities in the temperature range of 3.1 K to 300 K. The frequency and dephasing times of the phonons show anomalous temperature dependence below T_SC indicating a coupling of these low energy excitations with the Cooper-pair quasiparticles. A maximum in the amplitude of the acoustic modes at T ~ 170 is seen, attributed to spin fluctuations and strong spin-lattice coupling before T_SDW., Comment: 6 pages, 4 figures (revised manuscript)

We have studied the magnetism of the Pr3+ ions in PrFeAsO_1-xF_x (x = 0; 0.15) and its interaction with the Fe magnetic order (for x = 0). Specific heat data confirm the presence of a first excited crystal electric field (CEF) level around 3.5 meV in the undoped compound PrFeAsO. This finding is in agreement with recent neutron scattering experiments. The doped compound is found to have a much lower first CEF splitting of about 2.0 meV. The Pr ordering in PrFeAsO gives rise to large anomalies in the specific heat and the thermal expansion coefficient. In addition, a field-induced transition is found at low temperatures that is most pronounced for the magnetostriction coefficient. This transition, which is absent in the doped compound, is attributed to a reversal of the Fe spin canting as the antiferromagnetic Pr order is destroyed by the external magnetic field., Comment: 8 pages, 6 figures

Ac susceptibility and static magnetization measurements were performed in the nearly-optimally doped LaFeAsO$_{0.9}$F$_{0.1}$ and CeFeAsO$_{0.92}$F$_{0.08}$ superconductors, complementing earlier results on SmFeAsO$_{0.8}$F$_{0.2}$ [Phys. Rev. {\bf B 83}, 174514 (2011)]. The magnetic field -- temperature phase diagram of the mixed superconducting state is drawn for the three materials, displaying a sizeable reduction of the liquid phase upon increasing $T_{c}$ in the range of applied fields ($H \leq 5$ T). This result indicates that SmFeAsO$_{0.8}$F$_{0.2}$ is the most interesting compound among the investigated ones in view of possible applications. The field-dependence of the intra-grain depinning energy $U_{0}$ exhibits a common trend for all the samples with a typical crossover field value (2500 Oe $\lesssim H_{cr} \lesssim 5000$ Oe) separating regions where single and collective depinning processes are at work. Analysis of the data in terms of a simple two-fluid picture for slightly anisotropic materials allows to estimate the zero-temperature penetration depth $\lambda_{ab}(0)$ and the anisotropy parameter $\gamma$ for the three materials. Finally, a sizeable suppression of the superfluid density is deduced in a $s^{\pm}$ two-gap scenario.

Magnetic correlations in superconducting LiFeAs were studied by elastic and by inelastic neutron scattering experiments. There is no indication for static magnetic ordering but inelastic correlations appear at the incommensurate wave vector (0:5+-d 0:-+d 0) with d=0.07 slightly shifted from the commensurate ordering observed in other FeAs-based compounds. The incommensurate magnetic excitations respond to the opening of the superconducting gap by a transfer of spectral weight., 4 pages 5 figures