The recent discovery of superconductivity in oxypnictides with the critical temperature (TC) higher than McMillan limit of 39 K (the theoretical maximum predicted by Bardeen-Cooper-Schrieffer (BCS) theory) has generated great excitement. Theoretical calculations indicate that the electron-phonon interaction is not strong enough to give rise to such high transition temperatures, while strong ferromagnetic/antiferromagnetic fluctuations have been proposed to be responsible. However, superconductivity and magnetism in pnictide superconductors show a strong sensitivity to the lattice, suggesting a possibility of unconventional electron-phonon coupling. Here we report the effect of oxygen and iron isotopic mass on Tc and the spin-density wave (SDW) transition temperature (TSDW) in SmFeAsO1-xFx and Ba1-xKxFe2As2 systems. The results show that oxygen isotope effect on TC and TSDW is very little, while the iron isotope exponent alpha=-dlnTc/dlnM is about 0.35, being comparable to 0.5 for the full isotope effect. Surprisingly, the iron isotope exchange shows the same effect on TSDW as TCc These results indicate that electron-phonon interaction plays some role in the superconducting mechanism, but simple electron-phonon coupling mechanism seems to be rather unlikely because a strong magnon-phonon coupling is included. Sorting out the interplay between the lattice and magnetic degrees of freedom is a key challenge for understanding the mechanism of high-TC superconductivity.
Here we report the superconductivity in the iron-based oxyarsenide Sm[O1-xFx]FeAs, with the onset resistivity transition temperature at 55.0 K and Meissner transition at 54.6 K. This compound has the same crystal structure as LaOFeAs with shrunk crystal lattices, and becomes the superconductor with the highest critical temperature among all materials besides copper oxides.
We report on the synthesis and microstructural studies of fluorine based iron doped superconductors. We have successfully synthesized the fluorine based new superconducting material LaO1-xFxFeAs by choosing comparatively lower temperature and longer synthesis duration. The superconducting transition temperature that we have achieved is 27.5 K which is observed at doping level of x=0.2. The structural microstructural characterizations have been done by employing XRD, SEM and TEM techniques. The SEM and TEM micrographs reveal the layered structure.
The recently discovered superconducting - spin density wave materials, containing Fe and As, have raised huge interest. However most materials prepared to date, suffer from a varying degree of content of foreign Fe-As phases, Fe2As, FeAs2 and FeAs, which can lead to wrong conclusions concerning the properties of these materials. We show here that Mossbauer Spectroscopy is able to determine quite easily the relative content of the foreign phases. This procedure is demonstrated by a study of seven samples of superconducting or spin density wave materials, prepared in three different laboratories…
The recently discovered quaternary arsenide oxide superconductor La[O1-xFx]FeAs with the superconducting critical transition temperature (Tc) of 26 K [1], has been quickly expanded to another high-Tc superconducting system beyond copper oxides by the replacement of La with other rare earth elements, such as Sm, Ce, and Pr etc. [2-4], and the Pr[O1-xFx]FeAs has become to be the first non-cuprate superconductor that holding a Tc above 50 K. All these arsenide (including phosphide) superconductors formed in a same tetragonal layered structure with the space group P4/nmm which has an alternant sta…
Since the discovery of copper oxide superconductor in 1986 [1], extensive efforts have been devoted to the search of new high-Tc superconducting materials, especially high-Tc systems other than cuprates. The recently discovered quaternary superconductor La[O1-xFx]FeAs with the superconducting critical transition Tc of 26 K [2], which has a much simple layered structure compared with cuprates, has attracted quick enthusiasm and is going to become a new high-Tc system [3-6]. Here we report the discovery of bulk superconductivity in the praseodymium-arsenide oxides Pr[O1-xFx]FeAs with an onset dr…
75As-nuclear magnetic resonance (NMR) on an iron-based superconductor LaFeAsO1-xFx (x=0.14) was performed under a pressure of 3GPa. Enhancement of superconducting transition temperature Tc was confirmed from the relaxation rate 1/T1; Tc goes up to 40K by applying pressure up to 3GPa. 1/T1T, which is temperature independent just above Tc and gives a measure of the density of states (DOS) at the Fermi energy, enhances by applying pressure. These facts suggest that the increase of the DOS leads to the enhancement of Tc. On the other hand, anomalous behavior of 1/T1T observed at high temperatures …
The anisotropy of the nuclear spin-lattice relaxation rate $1/T_{1}$ of $^{75}$As was investigated in the iron-based superconductor LaFeAs(O$_{1-x}$F$_{x}$) ($x = 0.07, 0.11$ and 0.14) as well as LaFeAsO. While the temperature dependence of the normal-state $1/T_1T$ in the superconducting (SC) $x = 0.07$ is different from that in the SC $x = 0.11$, their anisotropy of $1/T_1$, $R \equiv (1/T_{1})_{H \parallel ab}/(1/T_{1})_{H \parallel c}$ in the normal state is almost the same ($\simeq$ 1.5). The observed anisotropy is ascribable to the presence of the local stripe correlations with $Q = (π, …
We use neutron scattering to study the structural and magnetic phase transitions in the iron pnictides CeFeAsO1-xFx as the system is tuned from a semimetal to a high-transition-temperature (high-Tc) superconductor through Fluorine (F) doping x. In the undoped state, CeFeAsO develops a structural lattice distortion followed by a stripe like commensurate antiferromagnetic order with decreasing temperature. With increasing Fluorine doping, the structural phase transition decreases gradually while the antiferromagnetic order is suppressed before the appearance of superconductivity, resulting an el…
The phenomenology of iron-pnictides superconductors can be explained in the framework of a three bands s\pm wave Eliashberg theory with only two free parameters plus a feedback effect i.e. the effect of the condensate on the antiferromagnetic spin fluctuactions responsible of the superconductivity in these compounds. I have examined the experimental data of four materials: LaFeAsO1-xFx, SmFeAsO1-xFx, Ba1-xKxFe2As2, and Ba(FexCo1-x)2As2 and I have found that it is possible to reproduce the experimental critical temperature and gap values in a moderate strong-coupling regime: ltot about 1.7-2.0.
In high-transition temperature (high-Tc) copper oxides, it is generally believed that antiferromagnetism plays a fundamental role in the superconducting mechanism because superconductivity occurs when mobile electrons or holes are doped into the antiferromagnetic parent compounds. The recent discovery of superconductivity in the rare-earth (R) iron-based oxide systems [RO1-xFxFeAs] has generated enormous interest because these materials are the first noncopper oxide superconductors with Tc exceeding 50 K. The parent (nonsuperconducting) LaOFeAs material is metallic but shows anomalies near 150…
The competition of magnetic order and superconductivity is a key element in the physics of all unconventional superconductors, e.g. in high-transition-temperature cuprates 1, heavy fermions 2 and organic superconductors3. Here superconductivity is often found close to a quantum critical point where long-range antiferromagnetic order is gradually suppressed as a function of a control parameter, e.g. charge carrier doping or pressure. It is believed that dynamic spin fluctuations associated with this quantum critical behaviour are crucial for the mechanism of superconductivity. Recently high-tem…
We report about muSR measurements on SmFeAsO1-xFx which helped us to identify the signature of diluted ferromagnetic inclusions, ubiquitous in the iron pnictides. These impurities are characterized by a Curie temperature close to room temperature and they seem responsible for a non negligible magnetic relaxation of the implanted muons, that should not be confused with intrinsic pnictide properties.
Local structure of NdFeAsO$_{1-x}$F$_{x}$ ($x$=0.0, 0.05, 0.15 and 0.18) high temperature iron pnictide superconductor system is studied using arsenic $K$-edge extended x-ray absorption fine structure measurements as a function of temperature. Fe-As bondlength shows only a weak temperature and F-substitution dependence, consistent with the strong covalent nature of this bond. The temperature dependence of the mean-square relative-displacements of the Fe-As bondlength are well described by the correlated-Einstein model for all the samples, but with different Einstein-temperatures for the superc…
We succeeded in growing single crystalline SmFeAsO1-xFx with exceptionally high fluorine concentration by using a CsCl flux method. Comparing to conventional flux methods, this method can introduce about double the amount of fluorine into the oxygen site. The obtained single crystal shows the highest superconducting transition temperature (Tc = 57.5 K) in single crystalline iron pnictides. In addition, the residual resistivity ratio (RRR) is almost three times as large as that of previously reported single crystals. This suggests that our single crystals are suitable for investigation of the i…
Study of superconductivity in layered iron-based materials was initiated in 2006 by Hosono's group, and boosted in 2008 by the superconducting transition temperature, Tc, of 26 K in LaFeAsO1-xFx. Since then, enormous researches have been done on the materials, with Tc reaching as high as 55 K. Here, we review briefly experimental and theoretical results on atomic and electronic structures and magnetic and superconducting properties of FeAs-based superconductors and related compounds. We seek for clues for unconventional superconductivity in the materials.
The Phase diagram of SmFeAsO1-xFx in terms of x is exhibited in this study. SmFeAsO1-xFx from x = 0 to x = 0.3 were prepared by low temperature sintering with slow cooling. The low temperature sintering suppresses the formation of the amorphous FeAs, which is inevitably produced as an impurity by using high temperature sintering. Moreover, slow cooling is effective to obtain the high fluorine concentration. The compositional change from feedstock composition is quite small after this synthesis. We can reproducibly observe a record superconducting transition for an iron based superconductor at …
We present a theoretical ab-initio approach that allows us to explicitly calculate the superconducting transition temperatures (Tc) of the iron-based superconductors of LaFeAsO1-xFx, SmFeAsO1-xFx, NdFeAsO1-xFx, Ba1-xKxFe2As2, FeSe and LiFeAs that fit perfectly with the experiments. We consider recent evidence that electron-phonon coupling may have been underestimated previously, and a prediction that antiferromagnetism can greatly enhance electron-phonon coupling through localized iron d orbitals. We then include the contribution of these localized orbitals in a McMillan formalism. In addition…
Fluoride-doped iron-based oxypnictides containing rare-earth gadolinium (GdFeAsO0.8F0.2) and co-doping with yttrium (Gd0.8Y0.2FeAsO0.8F0.2) have been prepared via conventional solid state reaction at ambient pressure. The non-yttrium substituted oxypnictide show superconducting transition as high as 43.9 K from temperature dependent resistance measurements with the Meissner effect observed at a lower temperature of 40.8 K from temperature dependent magnetization measurements. By replacing a small amount of gadolinium with yttrium Tc was observed to be lowered by 10 K which might be caused by a…
We estimate the changes in lattice parameters due to iron isotope substitution in the iron-based high temperature superconductors using a variational calculation based on the anharmonicity of the Fe-As(Se) bond. For BaFe2As2 and 57Fe to 54$Fe substitution we find a c-axis expansion of 1 10^{-3}Å and in-plane a-axis contraction of 1 10^{-5}Å at 250K in good agreement with experimental values on (Ba,K)Fe2As2 for which a negative isotope exponent α=-\frac{d\ln T_c}{d\ln m}<0 was found [P.M. Shirage et al., Phys. Rev. Lett. 103, 257003 (2009)]. For FeSe in contrast we find an expansion for both a …
The role of electron-phonon interactions in iron-based superconductor is currently under debate with conflicting experimental reports on the isotope effect. To address this important issue, we employ the renormalization-group method to investigate the competition between electron-electron and electron-phonon interactions in these materials. The renormalization-group analysis shows that the ground state is a phonon-dressed unconventional superconductor: the dominant electronic interactions account for pairing mechanism while electron-phonon interactions are subdominant. Because of the phonon dr…
Iron arsenide superconductors based on the material LaFeAsO1-xFx are characterized by a two-dimensional Fermi surface (FS) consisting of hole and electron pockets yielding structural and antiferromagnetic transitions at x = 0. Electron doping by substituting O2- with F- suppresses these transitions and gives rise to superconductivity with a maximum Tc = 26 K at x = 0.1. However, the over-doped region cannot be accessed due to the poor solubility of F- above x = 0.2. Here we overcome this problem by doping LaFeAsO with hydrogen. We report the phase diagram of LaFeAsO1-xHx (x < 0.53) and, in add…
Within a minimal model for the iron-based superconductors in which itinerant electrons interact with a band of local moments, we derive a a general conclusion for multi-band superconductivity. In a multi-band superconductor, due to the Adler theorem, the inter-band scattering dominates the intra-band scattering at the long wave length limit as long as both interactions are induced by Goldstone boson (which is magnon in our case) and the transfered momentum is nonzero. Such kind of interaction leads to a well-known sigh-reversing superconductivity even if the inter-band and intra-band interacti…
We study the pairing mechanism in iron pnictide superconductors based on the five-orbital Hubbard-Holstein model. Due to Fe-ion oscillations, the s-wave superconducting (SC) state without sign reversal (s_{++}-wave state) is induced by orbital fluctuations by using realistic model parameters. The virtue of the present theory is that the famous empirical relation between Tc and the As-Fe-As bond angle is automatically explained, since the electron-phonon (e-ph) coupling that creates the orbital fluctuations is the strongest when the As$_4$-tetrahedron is regular. The negative iron isotope effec…
The fluorine-doped rare-earth iron oxyarsenides, REFeAsO1-xFx (RE =rare earth) have recently emerged as a new family of high-temperature superconductors with transition temperatures (Tc) as high as 55 K (refs 1-4). Early work has provided compelling evidence that the undoped parent materials exhibit spin-density-wave (SDW) antiferromagnetic order and undergo a structural phase transition from tetragonal to orthorhombic crystal symmetry upon cooling.5 Both the magnetic and structural instabilities are suppressed upon doping with fluoride ions before the appearance of superconductivity.6,7 Here …
In a recent paper Yanagisawa et al. [1] claim from a theoretical analysis of a multi-channel multi-band superconductor model that an inverse isotope exponent on the superconducting transition temperature Tc can be realized in iron-based superconductors. Simultaneously, a subgroup of the authors of Ref. 1 performed the corresponding isotope effect experiment on (Ba, K)Fe2As2 by investigating the iron isotope exchange effect on Tc [2]. In accordance with their theoretical analysis they indeed report an unusually large sign reversed isotope exponent of α \simeq -0.18(3) which is in strong contras…
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.
We report the iron (Fe) isotope effect on the transition temperature (Tc) in the oxygen-deficient SmFeAsO_{1-y}, a 50 K-class Fe-based superconductor. For the optimally-doped samples with Tc = 54 K, change of the Fe average atomic mass (MFe) causes a negligibly small shift in Tc, with the Fe isotope coefficient (alphaFe) as small as -0.024 \pm 0.015. This result contrasts with the finite, inverse isotope shift observed in optimally-doped (Ba,K)Fe2As2, indicating that the contribution of the electron-phonon interaction markedly differs between these two Fe-based high-Tc superconductors.
The Fe isotope effect (Fe-IE) on the transition temperature T_c and the crystal structure was studied in the Fe chalcogenide superconductor FeSe_1-x by means of magnetization and neutron powder diffraction (NPD). The substitution of natural Fe (containing \simeq 92% of ^{56}Fe) by its lighter ^{54}Fe isotope leads to a shift of T_c of 0.22(5)K corresponding to an Fe-IE exponent of α_Fe=0.81(15). Simultaneously, a small structural change with isotope substitution is observed by NDP which may contribute to the total Fe isotope shift of T_c.
The magnetic and transport behaviors of cerium substituted iron oxy-arsenide superconductor with x = 0.1 to 0.4 fluoride (F) doping have been investigated in this report. Temperature dependent susceptibility and resistivity measurements showed the 0.1 F-doped sample (CeFeAsO0.9F0.1) has a superconducting transition temperature (Tc) of around 30 K. With increasing doping beyond x = 0.2 Tc saturates to around 40 K. Temperature dependent susceptibility measured in different magnetic fields for the under-doped sample showed Meissner effect in low field and the diamagnetism is still visible up to 1…
NMR longitudinal relaxation rates 1/T1 and Knight shifts K have been measured for superconducting samples of LaFe1-yCoyAsO1-xFx with y=0.0 and 0.0075 and for a nonsuperconducting metallic sample with y=0.1, where the x values are always fixed at 0.11. The temperature (T) dependence the relaxation rates 1/T1 of the superconducting samples has been found to be markedly different from the behavior 1/T1 T^(2.5-3.0) reported by many groups in the entire T range measured (from the temperature immediately below the superconducting transition temperature Tc down to (0.1-0.2)Tc). The nonexistence of th…
Following the discovery of superconductivity in an iron-based arsenide LaO1-xFxFeAs with a superconducting transition temperature (Tc) of 26 K[1], Tc was pushed up surprisingly to above 40 K by either applying pressure[2] or replacing La with Sm[3], Ce[4], Nd[5] and Pr[6]. The maximum Tc has climbed to 55 K, observed in SmO1-xFxFeAs[7, 8] and SmFeAsO1-x[9]. The value of Tc was found to increase with decreasing lattice parameters in LnFeAsO1-xFx (Ln stands for the lanthanide elements) at an apparently optimal doping level. However, the F- doping in GdFeAsO is particularly difficult[10,11] due t…
The present work describes the theoretical analysis of isotope effect coefficient as a function of transition temperature in two orbital per site model Hamiltonian in iron based superconducting system. The expression of isotope effect coefficient has been computed numerically and self-consistently by employing Green's function technique within the BCS-mean-field approximation. It is observed that the isotope effect coefficient increases with the increase of the hybridization while with the increase in Coulomb interaction it starts decreasing. On increasing the carrier density per site in two o…
The Comment insists on the following: in our model it is assumed that the effective interactions have specific energy ranges within the single band with a cutoff at ω_1 for the phononic part and a range from ω_1 to ω_2 in the AF channel. Our reply is that we assume that V_i(k,k')\neq 0 if |ξ_k|<ω_i and |ξ_{k'}|<ω_i, and otherwise V_i(k,k')= 0 (i=1,2), as stated in our paper. This is the model of BCS type with two attractive interactions, and this assumption is the characteristic of the BCS approximation. The claim "the integration limits have been modified such that the AF channel mediated pai…
We present Raman measurements on the iron-pnictide superconductors CeFeAsO_{1-x}F_{x} and NdFeAsO{1-x}F_{x}. Modeling the Fe-As plane in terms of harmonic and a cubic anharmonic Fe-As interaction we calculate the temperature dependence of the energy and lifetime of the Raman active Fe B_{1g} mode and fit to the observed energy shift. The shifts and lifetimes are in good agreement with those measured also in other Raman studies which demonstrate that the phonon spectrum is well represented by phonon-phonon interactions without any significant electronic contribution. We also estimate the anharm…
Complete electronic phase diagram and enhanced superconductivity in fluorine-doped PrFeAsO1-xFx
Institute of High Pressure Physics (IHPP), Polish Academy of Sciences（波兰科学院高压物理研究所）；Faculty of Physics, Warsaw University of Technology（华沙理工大学物理学院）；Institute of Physics, Polish Academy of Sciences（波兰科学院物理研究所）
We report self-consistent calculations of the gap symmetry for the iron-based high-temperature superconductors using realistic small-q phonon mediated pairing potentials and four-band energy dispersions. When both electron and hole Fermi surface pockets are present, we obtain the nodeless $s_\pm$ state that was first encountered in a spin-fluctuations mechanism picture. Nodal gap structures such as $d_{x^2-y^2}$ and $s_\pm+d_{x^2-y^2}$ and even a p-wave triplet state, are accessible upon doping within our phononic mechanism. Our results resolve the conflict between phase sensitive experiments …
Raman spectroscopy is a very powerful probe to study the nature of quasi-particle excitations in condensed matter physics. The work presented in this thesis is focused on two different families of novel materials, namely the iron-based superconductors (FeBS), multiferroic oxides and double perovskite. Although the properties of these two systems are quite different, some comparison can still be drawn between them. For instance, in both of these systems magnetism plays a crucial role and intricate coupling between phononic, magnetic and orbital degrees of freedom is crucial to understand their …
Effects of high-pressure synthesis on phase formation and superconducting properties of PrFeAsO1-xFx
Institute of High Pressure Physics (IHPP), Polish Academy of Sciences（波兰科学院高压物理研究所）；Faculty of Physics, Warsaw University of Technology（华沙理工大学物理学院）；Institute of Physics, Polish Academy of Sciences（波兰科学院物理研究所）
In view of the recent experimental facts in the iron-pnictides, we make a proposal that the itinerant electrons and local moments are simultaneously present in such multiband materials. We study a minimal model composed of coupled itinerant electrons and local moments to illustrate how a consistent explanation of the experimental measurements can be obtained in the leading order approximation. In this mean-field approach, the spin-density-wave (SDW) order and superconducting pairing of the itinerant electrons are not directly driven by the Fermi surface nesting, but are mainly induced by their…
The 1111-type iron-based superconductor LnFeAsO1-xFx (Ln stands for lanthanide) is the first material with a Tc above 50 K, other than cuprate superconductors. Electron doping into LaFeAsO by H, rather than F, revealed a double-dome-shaped Tc-x diagram, with a first dome (SC1, 0.05<x<0.20) and a second dome (SC2, 0.2<x<0.5). Here, we report the Tc for the whole hydrogen-doping range in LaFeAsO1-xHx under pressures of up to 19 GPa. Tc rises to 52 K at 6 GPa for the Tc-valley composition between the two Tc domes. This is the first instance of the Tc exceeding 50 K in La-1111-type iron-based supe…
Chemical substitution during growth is a well-established method to manipulate electronic states of quantum materials, and leads to rich spectra of phase diagrams in cuprate and iron-based superconductors. Here we report a novel and generic strategy to achieve nonvolatile electron doping in series of (i.e. 11 and 122 structures) Fe-based superconductors by ionic liquid gating induced protonation at room temperature. Accumulation of protons in bulk compounds induces superconductivity in the parent compounds, and enhances the Tc largely in some superconducting ones. Furthermore, the existence of…
Since the discovery of superconductivity at 26 K in oxy-pnictide LaFeAsO1-xFx, enormous interests have been stimulated in the field of condensed matter physics and material sciences. Among the many kind of structures in the iron pnictide superconductors, FeSe with the PbO structure has received special attention since there is not poisonous pnictogen element in chemical composition and its structure is the simplest one. However, the superconducting transition temperature (Tc) in iron chalcogenide compounds is not enhanced as high as other iron pnictide superconductors under ambient pressure un…
The recent discovery of superconductivity with relatively high transition temperature Tc in the layered iron-based quaternary oxypnictides La[ O1-xFx] FeAs was a real surprise. The excitement generated can be seen by the number of subsequent works published within a very short period of time. Although there exists superconductivity in alloy that contains Fe element, LaOMPn (with M= Fe, Ni; and Pn=P and As) is the first system where Fe-element plays the key role to the occurrence of superconductivity. LaOMPn has a layered crystal structure with an Fe-based plane. It is quite natural to ask whet…
Fe-based superconductors were discovered in 2008. This discovery with T$_c$ values up to 56 K, generated a new belief in the field of superconductivity. Till its discovery, high temperature superconductivity in cuprates, created a prejudice that Cu-oxides are essential building blocks for a high temperature superconducting material. These Fe based superconductors do not contain Cu-O planes (some of the materials are even O free). It will be argued in this review, that these iron pnictide and chalcogenide (FePn/Ch) superconductors have Fe electrons at the Fermi surface together with an unusual …
The dream of room temperature superconductors has inspired intense research effort to find routes for enhancing the superconducting transition temperature (Tc). Therefore, single-layer FeSe on a SrTiO3 substrate, with its extraordinarily high Tc amongst all interfacial superconductors and iron based superconductors, is particularly interesting, but the mechanism underlying its high Tc has remained mysterious. Here we show through isotope effects that electrons in FeSe couple with the oxygen phonons in the substrate, and the superconductivity is enhanced linearly with the coupling strength atop…
