Superconductivity at 43 K in an iron-based layered compound LaO(1-x)F(x)FeAs

The iron- and nickel-based layered compounds LaOFeP (refs 1, 2) and LaONiP (ref. 3) have recently been reported to exhibit low-temperature superconducting phases with transition temperatures T(c) of 3 and 5 K, respectively. Furthermore, a large increase in the midpoint T(c) of up to approximately 26 K has been realized in the isocrystalline compound LaOFeAs on doping of fluoride ions at the O2- sites (LaO(1-x)F(x)FeAs). Experimental observations and theoretical studies suggest that these transitions are related to a magnetic instability, as is the case for most superconductors based on transition metals. In the copper-based high-temperature superconductors, as well as in LaOFeAs, an increase in T(c) is often observed as a result of carrier doping in the two-dimensional electronic structure through ion substitution in the surrounding insulating layers, suggesting that the application of external pressure should further increase T(c) by enhancing charge transfer between the insulating and conducting layers. The effects of pressure on these iron oxypnictide superconductors may be more prominent than those in the copper-based systems, because the As ion has a greater electronic polarizability, owing to the covalency of the Fe-As chemical bond, and, thus, is more compressible than the divalent O2- ion. Here we report that increasing the pressure causes a steep increase in the onset T(c) of F-doped LaOFeAs, to a maximum of approximately 43 K at approximately 4 GPa. With the exception of the copper-based high-T(c) superconductors, this is the highest T(c) reported to date. The present result, together with the great freedom available in selecting the constituents of isocrystalline materials with the general formula LnOTMPn (Ln, Y or rare-earth metal; TM, transition metal; Pn, group-V, 'pnicogen', element), indicates that the layered iron oxypnictides are promising as a new material platform for further exploration of high-temperature superconductivity.     

Superconductivity at 43 K in SmFeAsO1-xFx

Since the discovery of high-transition-temperature (high-T(c)) superconductivity in layered copper oxides, extensive effort has been devoted to exploring the origins of this phenomenon. A T(c) higher than 40 K (about the theoretical maximum predicted from Bardeen-Cooper-Schrieffer theory), however, has been obtained only in the copper oxide superconductors. The highest reported value for non-copper-oxide bulk superconductivity is T(c) = 39 K in MgB(2) (ref. 2). The layered rare-earth metal oxypnictides LnOFeAs (where Ln is La-Nd, Sm and Gd) are now attracting attention following the discovery of superconductivity at 26 K in the iron-based LaO(1-x)F(x)FeAs (ref. 3). Here we report the discovery of bulk superconductivity in the related compound SmFeAsO(1-x)F(x), which has a ZrCuSiAs-type structure. Resistivity and magnetization measurements reveal a transition temperature as high as 43 K. This provides a new material base for studying the origin of high-temperature superconductivity.     

A BCS-like gap in the superconductor SmFeAsO0.85F0.15

Since the discovery of superconductivity in the high-transition-temperature (high-T(c)) copper oxides two decades ago, it has been firmly established that the CuO(2) plane is essential for superconductivity and gives rise to a host of other very unusual properties. A new family of superconductors with the general composition of LaFeAsO(1-x)F(x) has recently been discovered and the conspicuous lack of the CuO(2) planes raises the tantalizing question of a different pairing mechanism in these oxypnictides. The superconducting gap (its magnitude, structure, and temperature dependence) is intimately related to pairing. Here we report the observation of a single gap in the superconductor SmFeAsO(0.85)F(0.15) with T(c) = 42 K as measured by Andreev spectroscopy. The gap value of 2Delta = 13.34 +/- 0.3 meV gives 2Delta/k(B)T(c) = 3.68 (where k(B) is the Boltzmann constant), close to the Bardeen-Cooper-Schrieffer (BCS) prediction of 3.53. The gap decreases with temperature and vanishes at T(c) in a manner consistent with the BCS prediction, but dramatically different from that of the pseudogap behaviour in the copper oxide superconductors. Our results clearly indicate a nodeless gap order parameter, which is nearly isotropic in size across different sections of the Fermi surface, and are not compatible with models involving antiferromagnetic fluctuations, strong correlations, the t-J model, and the like, originally designed for the high-T(c) copper oxides.     

Visualizing pair formation on the atomic scale in the high-Tc superconductor Bi2Sr2CaCu2O8+delta

Pairing of electrons in conventional superconductors occurs at the superconducting transition temperature T(c), creating an energy gap Delta in the electronic density of states (DOS). In the high-T(c) superconductors, a partial gap in the DOS exists for a range of temperatures above T(c) (ref. 2). A key question is whether the gap in the DOS above T(c) is associated with pairing, and what determines the temperature at which incoherent pairs form. Here we report the first spatially resolved measurements of gap formation in a high-T(c) superconductor, measured on Bi2Sr2CaCu2O8+delta samples with different T(c) values (hole concentration of 0.12 to 0.22) using scanning tunnelling microscopy. Over a wide range of doping from 0.16 to 0.22 we find that pairing gaps nucleate in nanoscale regions above T(c). These regions proliferate as the temperature is lowered, resulting in a spatial distribution of gap sizes in the superconducting state. Despite the inhomogeneity, we find that every pairing gap develops locally at a temperature T(p), following the relation 2Delta/k(B)T(p) = 7.9 +/- 0.5. At very low doping (< or =0.14), systematic changes in the DOS indicate the presence of another phenomenon, which is unrelated and perhaps competes with electron pairing. Our observation of nanometre-sized pairing regions provides the missing microscopic basis for understanding recent reports of fluctuating superconducting response above T(c) in hole-doped high-T(c) copper oxide superconductors.     

Zero-resistance states induced by electromagnetic-wave excitation in GaAs/AlGaAs heterostructures

The observation of vanishing electrical resistance in condensed matter has led to the discovery of new phenomena such as, for example, superconductivity, where a zero-resistance state can be detected in a metal below a transition temperature T(c) (ref. 1). More recently, quantum Hall effects were discovered from investigations of zero-resistance states at low temperatures and high magnetic fields in two-dimensional electron systems (2DESs). In quantum Hall systems and superconductors, zero-resistance states often coincide with the appearance of a gap in the energy spectrum. Here we report the observation of zero-resistance states and energy gaps in a surprising setting: ultrahigh-mobility GaAs/AlGaAs heterostructures that contain a 2DES exhibit vanishing diagonal resistance without Hall resistance quantization at low temperatures and low magnetic fields when the specimen is subjected to electromagnetic wave excitation. Zero-resistance-states occur about magnetic fields B = 4/5 Bf and B = 4/9 Bf, where Bf = 2pifm*/e,m* is the electron mass, e is the electron charge, and f is the electromagnetic-wave frequency. Activated transport measurements on the resistance minima also indicate an energy gap at the Fermi level. The results suggest an unexpected radiation-induced, electronic-state-transition in the GaAs/AlGaAs 2DES.     

Addition of nanoparticle dispersions to enhance flux pinning of the YBa2Cu3O7-x superconductor

Following the discovery of type-II high-temperature superconductors in 1986 (refs 1, 2), work has proceeded to develop these materials for power applications. One of the problems, however, has been that magnetic flux is not completely expelled, but rather is contained within magnetic fluxons, whose motion prevents larger supercurrents. It is known that the critical current of these materials can be enhanced by incorporating a high density of extended defects to act as pinning centres for the fluxons. YBa2Cu3O7 (YBCO or 123) is the most promising material for such applications at higher temperatures (liquid nitrogen). Pinning is optimized when the size of the defects approaches the superconducting coherence length ( approximately 2-4 nm for YBCO at temperatures < or =77 K) and when the areal number density of defects is of the order of (H/2) x 10(11) cm(-2), where H is the applied magnetic field in tesla. Such a high density has been difficult to achieve by material-processing methods that maintain a nanosize defect, except through irradiation. Here we report a method for achieving a dispersion of approximately 8-nm-sized nanoparticles in YBCO with a high number density, which increases the critical current (at 77 K) by a factor of two to three for high magnetic fields.     

The structure of the high-energy spin excitations in a high-transition-temperature superconductor

In conventional superconductors, lattice vibrations (phonons) mediate the attraction between electrons that is responsible for superconductivity. The high transition temperatures (high-T(c)) of the copper oxide superconductors has led to collective spin excitations being proposed as the mediating excitations in these materials. The mediating excitations must be strongly coupled to the conduction electrons, have energy greater than the pairing energy, and be present at T(c). The most obvious feature in the magnetic excitations of high-T(c) superconductors such as YBa2Cu3O6+x is the so-called 'resonance'. Although the resonance may be strongly coupled to the superconductivity, it is unlikely to be the main cause, because it has not been found in the La2-x(Ba,Sr)(x)CuO4 family and is not universally present in Bi2Sr2CaCu2O8+delta (ref. 9). Here we use inelastic neutron scattering to characterize possible mediating excitations at higher energies in YBa2Cu3O6.6. We observe a square-shaped continuum of excitations peaked at incommensurate positions. These excitations have energies greater than the superconducting pairing energy, are present at T(c), and have spectral weight far exceeding that of the 'resonance'. The discovery of similar excitations in La2-xBa(x)CuO4 (ref. 10) suggests that they are a general property of the copper oxides, and a candidate for mediating the electron pairing.     

Resonance as a measure of pairing correlations in the high-Tc superconductor YBa2Cu3O6.6

One of the most striking properties of the high-transition-temperature (high-Tc) superconductors is that they are all derived from insulating antiferromagnetic parent compounds. The intimate relationship between magnetism and superconductivity in these copper oxide materials has intrigued researchers from the outset, because it does not exist in conventional superconductors. Evidence for this link comes from neutron-scattering experiments that show the unambiguous presence of short-range antiferromagnetic correlations (excitations) in the high-Tc superconductors. Even so, the role of such excitations in the pairing mechanism for superconductivity is still a subject of controversy. For YBa2Cu3O(6+x), where x controls the hole-doping level, the most prominent feature in the magnetic excitation spectrum is a sharp resonance (refs 6-11). Here we show that for underdoped YBa2Cu3O6.6, where x and Tc are below their optimal values, modest magnetic fields suppress the resonance significantly, much more so for fields approximately perpendicular to the CuO2 planes than for parallel fields. Our results indicate that the resonance measures pairing and phase coherence, suggesting that magnetism plays an important role in high-Tc superconductivity. The persistence of a field effect above Tc favours mechanisms in which the superconducting electron pairs are pre-formed in the normal state of underdoped copper oxide superconductors, awaiting transition to the superconducting state.     

High critical current density and enhanced irreversibility field in superconducting MgB2 thin films

The discovery of superconductivity at 39 K in magnesium diboride offers the possibility of a new class of low-cost, high-performance superconducting materials for magnets and electronic applications. This compound has twice the transition temperature of Nb3Sn and four times that of Nb-Ti alloy, and the vital prerequisite of strongly linked current flow has already been demonstrated. One possible drawback, however, is that the magnetic field at which superconductivity is destroyed is modest. Furthermore, the field which limits the range of practical applications-the irreversibility field H*(T)-is approximately 7 T at liquid helium temperature (4.2 K), significantly lower than about 10 T for Nb-Ti (ref. 6) and approximately 20 T for Nb3Sn (ref. 7). Here we show that MgB2 thin films that are alloyed with oxygen can exhibit a much steeper temperature dependence of H*(T) than is observed in bulk materials, yielding an H* value at 4.2 K greater than 14 T. In addition, very high critical current densities at 4.2 K are achieved: 1 MA cm-2 at 1 T and 105 A cm-2 at 10 T. These results demonstrate that MgB2 has potential for high-field superconducting applications.     

Diamagnetic activity above Tc as a precursor to superconductivity in La2-xSrxCuO4 thin films

Superconductors show zero resistance to electric current, and expel magnetic flux (the Meissner effect) below the transition temperature (Tc). In conventional superconductors, the 'Cooper pairs' of electrons that are responsible for superconductivity form only below Tc. In the unconventional high-Tc superconductors, however, a strong electron correlation is essential for pair formation: there is evidence that some pairs are formed above Tc in samples that have less than the optimal density of charge carriers (underdoped) and an energy gap-the 'pseudogap'-appears to be present. Moreover, excitations that look like the vortices that carry magnetic flux inside the superconducting state have been reported above Tc (refs 6, 7). Although the origin of the pseudogap remains controversial, phase fluctuations above Tc, leading to some form of local superconductivity or local pairing, seem essential. Here we report magnetic imaging (scanning SQUID microscopy) of La2-xSrxCuO4 thin films. Clear quantized vortex patterns are visible below Tc (18-19 K), and we observe inhomogeneous magnetic domains that persist up to 80 K. We interpret the data as suggesting the existence of diamagnetic regions that are precursors to the Meissner state.     

Resonance in the electron-doped high-transition-temperature superconductor Pr0.88LaCe0.12CuO4-delta

In conventional superconductors, the interaction that pairs the electrons to form the superconducting state is mediated by lattice vibrations (phonons). In high-transition-temperature (high-T(c)) copper oxides, it is generally believed that magnetic excitations might play a fundamental role in the superconducting mechanism because superconductivity occurs when mobile 'electrons' or 'holes' are doped into the antiferromagnetic parent compounds. Indeed, a sharp magnetic excitation termed 'resonance' has been observed by neutron scattering in a number of hole-doped materials. The resonance is intimately related to superconductivity, and its interaction with charged quasi-particles observed by photoemission, optical conductivity, and tunnelling suggests that it might play a part similar to that of phonons in conventional superconductors. The relevance of the resonance to high-T(c) superconductivity, however, has been in doubt because so far it has been found only in hole-doped materials. Here we report the discovery of the resonance in electron-doped superconducting Pr0.88LaCe0.12CuO4-delta (T(c) = 24 K). We find that the resonance energy (E(r)) is proportional to T(c) via E(r) approximately 5.8k(B)T(c) for all high-T(c) superconductors irrespective of electron- or hole-doping. Our results demonstrate that the resonance is a fundamental property of the superconducting copper oxides and therefore must be essential in the mechanism of superconductivity.     

Electronic structure of the iron-based superconductor LaOFeP

The recent discovery of superconductivity in the iron oxypnictide family of compounds has generated intense interest. The layered crystal structure with transition-metal ions in planar square-lattice form and the discovery of spin-density-wave order near 130 K (refs 10, 11) seem to hint at a strong similarity with the copper oxide superconductors. An important current issue is the nature of the ground state of the parent compounds. Two distinct classes of theories, distinguished by the underlying band structure, have been put forward: a local-moment antiferromagnetic ground state in the strong-coupling approach, and an itinerant ground state in the weak-coupling approach. The first approach stresses on-site correlations, proximity to a Mott-insulating state and, thus, the resemblance to the high-transition-temperature copper oxides, whereas the second approach emphasizes the itinerant-electron physics and the interplay between the competing ferromagnetic and antiferromagnetic fluctuations. The debate over the two approaches is partly due to the lack of conclusive experimental information on the electronic structures. Here we report angle-resolved photoemission spectroscopy (ARPES) of LaOFeP (superconducting transition temperature, T(c) = 5.9 K), the first-reported iron-based superconductor. Our results favour the itinerant ground state, albeit with band renormalization. In addition, our data reveal important differences between these and copper-based superconductors.     

Abrupt onset of a second energy gap at the superconducting transition of underdoped Bi2212

The superconducting gap--an energy scale tied to the superconducting phenomena--opens on the Fermi surface at the superconducting transition temperature (T(c)) in conventional BCS superconductors. In underdoped high-T(c) superconducting copper oxides, a pseudogap (whose relation to the superconducting gap remains a mystery) develops well above T(c) (refs 1, 2). Whether the pseudogap is a distinct phenomenon or the incoherent continuation of the superconducting gap above T(c) is one of the central questions in high-T(c) research. Although some experimental evidence suggests that the two gaps are distinct, this issue is still under intense debate. A crucial piece of evidence to firmly establish this two-gap picture is still missing: a direct and unambiguous observation of a single-particle gap tied to the superconducting transition as function of temperature. Here we report the discovery of such an energy gap in underdoped Bi2Sr2CaCu2O8+delta in the momentum space region overlooked in previous measurements. Near the diagonal of Cu-O bond direction (nodal direction), we found a gap that opens at T(c) and has a canonical (BCS-like) temperature dependence accompanied by the appearance of the so-called Bogoliubov quasi-particles, a classical signature of superconductivity. This is in sharp contrast to the pseudogap near the Cu-O bond direction (antinodal region) measured in earlier experiments.     

Superconductivity at 39 K in magnesium diboride

In the light of the tremendous progress that has been made in raising the transition temperature of the copper oxide superconductors (for a review, see ref. 1), it is natural to wonder how high the transition temperature, Tc, can be pushed in other classes of materials. At present, the highest reported values of Tc for non-copper-oxide bulk superconductivity are 33 K in electron-doped Cs(x)Rb(y)C60 (ref. 2), and 30 K in Ba(1-x)K(x)BiO3 (ref. 3). (Hole-doped C60 was recently found to be superconducting with a Tc as high as 52 K, although the nature of the experiment meant that the supercurrents were confined to the surface of the C60 crystal, rather than probing the bulk.) Here we report the discovery of bulk superconductivity in magnesium diboride, MgB2. Magnetization and resistivity measurements establish a transition temperature of 39 K, which we believe to be the highest yet determined for a non-copper-oxide bulk superconductor.     

Re-emerging superconductivity at 48 kelvin in iron chalcogenides

Pressure has an essential role in the production and control of superconductivity in iron-based superconductors. Substitution of a large cation by a smaller rare-earth ion to simulate the pressure effect has raised the superconducting transition temperature T(c) to a record high of 55?K in these materials. In the same way as T(c) exhibits a bell-shaped curve of dependence on chemical doping, pressure-tuned T(c) typically drops monotonically after passing the optimal pressure. Here we report that in the superconducting iron chalcogenides, a second superconducting phase suddenly re-emerges above 11.5?GPa, after the T(c) drops from the first maximum of 32?K at 1?GPa. The T(c) of the re-emerging superconducting phase is considerably higher than the first maximum, reaching 48.0-48.7?K for Tl(0.6)Rb(0.4)Fe(1.67)Se(2), K(0.8)Fe(1.7)Se(2) and K(0.8)Fe(1.78)Se(2).     

A hidden pseudogap under the 'dome' of superconductivity in electron-doped high-temperature superconductors

The ground state of superconductors is characterized by the long-range order of condensed Cooper pairs: this is the only order present in conventional superconductors. The high-transition-temperature (high-T(c)) superconductors, in contrast, exhibit more complex phase behaviour, which might indicate the presence of other competing ground states. For example, the pseudogap--a suppression of the accessible electronic states at the Fermi level in the normal state of high-T(c) superconductors-has been interpreted as either a precursor to superconductivity or as tracer of a nearby ground state that can be separated from the superconducting state by a quantum critical point. Here we report the existence of a second order parameter hidden within the superconducting phase of the underdoped (electron-doped) high-T(c) superconductor Pr2-xCe(x)CuO4-y and the newly synthesized electron-doped material La2-xCe(x)CuO4-y (ref. 8). The existence of a pseudogap when superconductivity is suppressed excludes precursor superconductivity as its origin. Our observation is consistent with the presence of a (quantum) phase transition at T = 0, which may be a key to understanding high-T(c) superconductivity. This supports the picture that the physics of high-T(c) superconductors is determined by the interplay between competing and coexisting ground states.     

Superconductivity in the non-oxide perovskite MgCNi3

The interplay of magnetic interactions, the dimensionality of the crystal structure and electronic correlations in producing superconductivity is one of the dominant themes in the study of the electronic properties of complex materials. Although magnetic interactions and two-dimensional structures were long thought to be detrimental to the formation of a superconducting state, they are actually common features of both the high transition-temperature (Tc) copper oxides and low-Tc material Sr2RuO4, where they appear to be essential contributors to the exotic electronic states of these materials. Here we report that the perovskite-structured compound MgCNi3 is superconducting with a critical temperature of 8 K. This material is the three-dimensional analogue of the LnNi2B2C family of superconductors, which have critical temperatures up to 16 K (ref. 2). The itinerant electrons in both families of materials arise from the partial filling of the nickel d-states, which generally leads to ferromagnetism as is the case in metallic Ni. The high relative proportion of Ni in MgCNi3 suggests that magnetic interactions are important, and the lower Tc of this three-dimensional compound-when compared to the LnNi2B2C family-contrasts with conventional ideas regarding the origins of superconductivity.     

Superconductivity in single crystals of the fullerene C70.

The observation of superconductivity in doped C60 has attracted much attention, as these materials represent an entirely new class of superconductors. A maximum transition temperature (Tc) of 40 K has been reported for electron-doped C60 crystals, while a Tc of 52 K has been seen in hole-doped crystals; only the copper oxide superconductors have higher transition temperatures. The results for C60 raise the intriguing questions of whether conventional electron-phonon coupling alone can produce such high transition temperatures, and whether even higher transition temperatures might be observed in other fullerenes. There have, however, been no confirmed reports of superconductivity in other fullerenes, though it has recently been observed in carbon nanotubes. Here we report the observation of superconductivity in single crystals of electric-field-doped C70. The maximum transition temperature of about 7 K is achieved when the sample is doped to approximately four electrons per C70 molecule, which corresponds to a half-filled conduction band. We anticipate superconductivity in smaller fullerenes at temperatures even higher than in C60 if the right charge density can be induced.     

Spontaneous breaking of time-reversal symmetry in the pseudogap state of a high-Tc superconductor

A change in 'symmetry' is often observed when matter undergoes a phase transition-the symmetry is said to be spontaneously broken. The transition made by underdoped high-transition-temperature (high-Tc) superconductors is unusual, in that it is not a mean-field transition as seen in other superconductors. Rather, there is a region in the phase diagram above the superconducting transition temperature Tc (where phase coherence and superconductivity begin) but below a characteristic temperature T* where a 'pseudogap' appears in the spectrum of electronic excitations. It is therefore important to establish if T* is just a cross-over temperature arising from fluctuations in the order parameter that will establish superconductivity at Tc (refs 3, 4), or if it marks a phase transition where symmetry is spontaneously broken. Here we report that, for a material in the pseudogap state, left-circularly polarized photons give a different photocurrent from right-circularly polarized photons. This shows that time-reversal symmetry is spontaneously broken below T*, which therefore corresponds to a phase transition.     

Pressure-induced crystallization of a spin liquid

Liquids are expected to crystallize at low temperature. The only exception is helium, which can remain liquid at 0 K, owing to quantum fluctuations. Similarly, the atomic magnetic moments (spins) in a magnet are expected to order at a temperature scale set by the Curie-Weiss temperature theta(CW) (ref. 3). Geometrically frustrated magnets represent an exception. In these systems, the pairwise spin interactions cannot be simultaneously minimized because of the lattice symmetry. This can stabilize a liquid-like state of short-range-ordered fluctuating moments well below theta(CW) (refs 5-7). Here we use neutron scattering to observe the spin liquid state in a geometrically frustrated system, Tb(2)Ti(2)O(7), under conditions of high pressure (approximately 9 GPa) and low temperature (approximately 1 K). This compound is a three-dimensional magnet with theta(CW) = -19 K, where the negative value indicates antiferromagnetic interactions. At ambient pressure Tb(2)Ti(2)O(7) remains in a spin liquid state down to at least 70 mK (ref. 8). But we find that, under high pressure, the spins start to order or 'crystallize' below 2.1 K, with antiferromagnetic order coexisting with liquid-like fluctuations. These results indicate that a spin liquid/solid mixture can be induced by pressure in geometrically frustrated systems.