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.     

Two-dimensional geometry of spin excitations in the high-transition-temperature superconductor YBa2Cu3O6+x

The fundamental building block of the copper oxide superconductors is a Cu4O4 square plaquette. The plaquettes in most of these materials are slightly distorted to form a rectangular lattice, for which an influential theory predicts that high-transition-temperature (high-T(c)) superconductivity is nucleated in 'stripes' aligned along one of the axes. This theory received strong support from experiments that indicated a one-dimensional character for the magnetic excitations in the high-T(c) material YBa2Cu3O6.6 (ref. 4). Here we report neutron scattering data on 'untwinned' YBa2Cu3O6+x crystals, in which the orientation of the rectangular lattice is maintained throughout the entire volume. Contrary to the earlier claim, we demonstrate that the geometry of the magnetic fluctuations is two-dimensional. Rigid stripe arrays therefore appear to be ruled out over a wide range of doping levels in YBa2Cu3O6+x, but the data may be consistent with liquid-crystalline stripe order. The debate about stripes has therefore been reopened.     

Magnetic-field-induced charge-stripe order in the high-temperature superconductor YBa2Cu3Oy

Electronic charges introduced in copper-oxide (CuO(2)) planes generate high-transition-temperature (T(c)) superconductivity but, under special circumstances, they can also order into filaments called stripes. Whether an underlying tendency towards charge order is present in all copper oxides and whether this has any relationship with superconductivity are, however, two highly controversial issues. To uncover underlying electronic order, magnetic fields strong enough to destabilize superconductivity can be used. Such experiments, including quantum oscillations in YBa(2)Cu(3)O(y) (an extremely clean copper oxide in which charge order has not until now been observed) have suggested that superconductivity competes with spin, rather than charge, order. Here we report nuclear magnetic resonance measurements showing that high magnetic fields actually induce charge order, without spin order, in the CuO(2) planes of YBa(2)Cu(3)O(y). The observed static, unidirectional, modulation of the charge density breaks translational symmetry, thus explaining quantum oscillation results, and we argue that it is most probably the same 4a-periodic modulation as in stripe-ordered copper oxides. That it develops only when superconductivity fades away and near the same 1/8 hole doping as in La(2-x)Ba(x)CuO(4) (ref.?1) suggests that charge order, although visibly pinned by CuO chains in YBa(2)Cu(3)O(y), is an intrinsic propensity of the superconducting planes of high-T(c) copper oxides.     

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.     

Electron pockets in the Fermi surface of hole-doped high-Tc superconductors

High-temperature superconductivity in copper oxides occurs when the materials are chemically tuned to have a carrier concentration intermediate between their metallic state at high doping and their insulating state at zero doping. The underlying evolution of the electron system in the absence of superconductivity is still unclear, and a question of central importance is whether it involves any intermediate phase with broken symmetry. The Fermi surface of the electronic states in the underdoped 'YBCO' materials YBa2Cu3O(y) and YBa2Cu4O8 was recently shown to include small pockets, in contrast with the large cylinder that characterizes the overdoped regime, pointing to a topological change in the Fermi surface. Here we report the observation of a negative Hall resistance in the magnetic-field-induced normal state of YBa2Cu3O(y) and YBa2Cu4O8, which reveals that these pockets are electron-like rather than hole-like. We propose that these electron pockets most probably arise from a reconstruction of the Fermi surface caused by the onset of a density-wave phase, as is thought to occur in the electron-doped copper oxides near the onset of antiferromagnetic order. Comparison with materials of the La2CuO4 family that exhibit spin/charge density-wave order suggests that a Fermi surface reconstruction also occurs in those materials, pointing to a generic property of high-transition-temperature (T(c)) superconductors.     

Quantum oscillations and the Fermi surface in an underdoped high-Tc superconductor

Despite twenty years of research, the phase diagram of high-transition-temperature superconductors remains enigmatic. A central issue is the origin of the differences in the physical properties of these copper oxides doped to opposite sides of the superconducting region. In the overdoped regime, the material behaves as a reasonably conventional metal, with a large Fermi surface. The underdoped regime, however, is highly anomalous and appears to have no coherent Fermi surface, but only disconnected 'Fermi arcs'. The fundamental question, then, is whether underdoped copper oxides have a Fermi surface, and if so, whether it is topologically different from that seen in the overdoped regime. Here we report the observation of quantum oscillations in the electrical resistance of the oxygen-ordered copper oxide YBa2Cu3O6.5, establishing the existence of a well-defined Fermi surface in the ground state of underdoped copper oxides, once superconductivity is suppressed by a magnetic field. The low oscillation frequency reveals a Fermi surface made of small pockets, in contrast to the large cylinder characteristic of the overdoped regime. Two possible interpretations are discussed: either a small pocket is part of the band structure specific to YBa2Cu3O6.5 or small pockets arise from a topological change at a critical point in the phase diagram. Our understanding of high-transition-temperature (high-T(c)) superconductors will depend critically on which of these two interpretations proves to be correct.     

Superconductivity in two-dimensional CoO2 layers

Since the discovery of high-transition-temperature (high-T(c)) superconductivity in layered copper oxides, many researchers have searched for similar behaviour in other layered metal oxides involving 3d-transition metals, such as cobalt and nickel. Such attempts have so far failed, with the result that the copper oxide layer is thought to be essential for superconductivity. Here we report that Na(x)CoO2*yH2O (x approximately 0.35, y approximately 1.3) is a superconductor with a T(c) of about 5 K. This compound consists of two-dimensional CoO2 layers separated by a thick insulating layer of Na+ ions and H2O molecules. There is a marked resemblance in superconducting properties between the present material and high-T(c) copper oxides, suggesting that the two systems have similar underlying physics.     

Link between spin fluctuations and electron pairing in copper oxide superconductors

Although it is generally accepted that superconductivity is unconventional in the high-transition-temperature copper oxides, the relative importance of phenomena such as spin and charge (stripe) order, superconductivity fluctuations, proximity to a Mott insulator, a pseudogap phase and quantum criticality are still a matter of debate. In electron-doped copper oxides, the absence of an anomalous pseudogap phase in the underdoped region of the phase diagram and weaker electron correlations suggest that Mott physics and other unidentified competing orders are less relevant and that antiferromagnetic spin fluctuations are the dominant feature. Here we report a study of magnetotransport in thin films of the electron-doped copper oxide La(2?-?x)Ce(x)CuO(4). We show that a scattering rate that is linearly dependent on temperature--a key feature of the anomalous normal state properties of the copper oxides--is correlated with the electron pairing. We also show that an envelope of such scattering surrounds the superconducting phase, surviving to zero temperature when superconductivity is suppressed by magnetic fields. Comparison with similar behaviour found in organic superconductors strongly suggests that the linear dependence on temperature of the resistivity in the electron-doped copper oxides is caused by spin-fluctuation scattering.     

An hour-glass magnetic spectrum in an insulating, hole-doped antiferromagnet

Superconductivity in layered copper oxide compounds emerges when charge carriers are added to antiferromagnetically ordered CuO(2) layers. The carriers destroy the antiferromagnetic order, but strong spin fluctuations persist throughout the superconducting phase and are intimately linked to superconductivity. Neutron scattering measurements of spin fluctuations in hole-doped copper oxides have revealed an unusual 'hour-glass' feature in the momentum-resolved magnetic spectrum that is present in a wide range of superconducting and non-superconducting materials. There is no widely accepted explanation for this feature. One possibility is that it derives from a pattern of alternating spin and charge stripes, and this idea is supported by measurements on stripe-ordered La(1.875)Ba(0.125)CuO(4) (ref. 15). Many copper oxides without stripe order, however, also exhibit an hour-glass spectrum. Here we report the observation of an hour-glass magnetic spectrum in a hole-doped antiferromagnet from outside the family of superconducting copper oxides. Our system has stripe correlations and is an insulator, which means that its magnetic dynamics can conclusively be ascribed to stripes. The results provide compelling evidence that the hour-glass spectrum in the copper oxide superconductors arises from fluctuating stripes.     

Magnetic order close to superconductivity in the iron-based layered LaO1-xFxFeAs systems

Following the discovery of long-range antiferromagnetic order in the parent compounds of high-transition-temperature (high-T(c)) copper oxides, there have been efforts to understand the role of magnetism in the superconductivity that occurs when mobile 'electrons' or 'holes' are doped into the antiferromagnetic parent compounds. Superconductivity in the newly discovered rare-earth iron-based oxide systems ROFeAs (R, rare-earth metal) also arises from either electron or hole doping of their non-superconducting parent compounds. The parent material LaOFeAs is metallic but shows anomalies near 150 K in both resistivity and d.c. magnetic susceptibility. Although optical conductivity and theoretical calculations suggest that LaOFeAs exhibits a spin-density-wave (SDW) instability that is suppressed by doping with electrons to induce superconductivity, there has been no direct evidence of SDW order. Here we report neutron-scattering experiments that demonstrate that LaOFeAs undergoes an abrupt structural distortion below 155 K, changing the symmetry from tetragonal (space group P4/nmm) to monoclinic (space group P112/n) at low temperatures, and then, at approximately 137 K, develops long-range SDW-type antiferromagnetic order with a small moment but simple magnetic structure. Doping the system with fluorine suppresses both the magnetic order and the structural distortion in favour of superconductivity. Therefore, like high-T(c) copper oxides, the superconducting regime in these iron-based materials occurs in close proximity to a long-range-ordered antiferromagnetic ground state.     

Antiferromagnetic order induced by an applied magnetic field in a high-temperature superconductor.

One view of the high-transition-temperature (high-Tc) copper oxide superconductors is that they are conventional superconductors where the pairing occurs between weakly interacting quasiparticles (corresponding to the electrons in ordinary metals), although the theory has to be pushed to its limit. An alternative view is that the electrons organize into collective textures (for example, charge and spin stripes) which cannot be 'mapped' onto the electrons in ordinary metals. Understanding the properties of the material would then need quantum field theories of objects such as textures and strings, rather than point-like electrons. In an external magnetic field, magnetic flux penetrates type II superconductors via vortices, each carrying one flux quantum. The vortices form lattices of resistive material embedded in the non-resistive superconductor, and can reveal the nature of the ground state-for example, a conventional metal or an ordered, striped phase-which would have appeared had superconductivity not intervened, and which provides the best starting point for a pairing theory. Here we report that for one high-Tc superconductor, the applied field that imposes the vortex lattice also induces 'striped' antiferromagnetic order. Ordinary quasiparticle models can account for neither the strength of the order nor the nearly field-independent antiferromagnetic transition temperature observed in our measurements.     

A multi-component Fermi surface in the vortex state of an underdoped high-Tc superconductor

To understand the origin of superconductivity, it is crucial to ascertain the nature and origin of the primary carriers available to participate in pairing. Recent quantum oscillation experiments on high-transition-temperature (high-T(c)) copper oxide superconductors have revealed the existence of a Fermi surface akin to that in normal metals, comprising fermionic carriers that undergo orbital quantization. The unexpectedly small size of the observed carrier pocket, however, leaves open a variety of possibilities for the existence or form of any underlying magnetic order, and its relation to d-wave superconductivity. Here we report experiments on quantum oscillations in the magnetization (the de Haas-van Alphen effect) in superconducting YBa(2)Cu(3)O(6.51) that reveal more than one carrier pocket. In particular, we find evidence for the existence of a much larger pocket of heavier mass carriers playing a thermodynamically dominant role in this hole-doped superconductor. Importantly, characteristics of the multiple pockets within this more complete Fermi surface impose constraints on the wavevector of any underlying order and the location of the carriers in momentum space. These constraints enable us to construct a possible density-wave model with spiral or related modulated magnetic order, consistent with experimental observations.     

Negative lattice expansion from the superconductivity--antiferromagnetism crossover in ruthenium copper oxides

The mechanism of high-transition-temperature (high-T(c)) superconductivity in doped copper oxides is an enduring problem. Antiferromagnetism is established as the competing order, but the relationship between the two states in the intervening 'pseudogap' regime has become a central puzzle. The role of the crystal lattice, which is important in conventional superconductors, also remains unclear. Here we report an anomalous increase of the distance between copper oxide planes on cooling, which results in negative thermal volume expansion, for layered ruthenium copper oxides that have been doped to the boundary of antiferromagnetism and superconductivity. We propose that a crossover between these states is driven by spin ordering in the ruthenium oxide layers, revealing a novel mechanism for negative lattice expansion in solids. The differences in volume and lattice strain between the distinct superconducting and antiferromagnetic states can account for the phase segregation phenomena found extensively in low-doped copper oxides, and show that Cooper pair formation is coupled to the lattice. Unusually large variations of resistivity with magnetic field are found in these ruthenium copper oxides at low temperatures through coupling between the ordered Ru and Cu spins.     

High-transition-temperature superconductivity in the absence of the magnetic-resonance mode

The fundamental mechanism that gives rise to high-transition-temperature (high-T(c)) superconductivity in the copper oxide materials has been debated since the discovery of the phenomenon. Recent work has focused on a sharp 'kink' in the kinetic energy spectra of the electrons as a possible signature of the force that creates the superconducting state. The kink has been related to a magnetic resonance and also to phonons. Here we report that infrared spectra of Bi2Sr2CaCu2O8+delta (Bi-2212), shows that this sharp feature can be separated from a broad background and, interestingly, weakens with doping before disappearing completely at a critical doping level of 0.23 holes per copper atom. Superconductivity is still strong in terms of the transition temperature at this doping (T(c) approximately 55 K), so our results rule out both the magnetic resonance peak and phonons as the principal cause of high-T(c) superconductivity. The broad background, on the other hand, is a universal property of the copper-oxygen plane and provides a good candidate signature of the 'glue' that binds the electrons.     

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.     

Crystallization of charge holes in the spin ladder of Sr14Cu24O41

Determining the nature of the electronic phases that compete with superconductivity in high-transition-temperature (high-T(c)) superconductors is one of the deepest problems in condensed matter physics. One candidate is the 'stripe' phase, in which the charge carriers (holes) condense into rivers of charge that separate regions of antiferromagnetism. A related but lesser known system is the 'spin ladder', which consists of two coupled chains of magnetic ions forming an array of rungs. A doped ladder can be thought of as a high-T(c) material with lower dimensionality, and has been predicted to exhibit both superconductivity and an insulating 'hole crystal' phase in which the carriers are localized through many-body interactions. The competition between the two resembles that believed to operate between stripes and superconductivity in high-T(c) materials. Here we report the existence of a hole crystal in the doped spin ladder of Sr14Cu24O41 using a resonant X-ray scattering technique. This phase exists without a detectable distortion in the structural lattice, indicating that it arises from many-body electronic effects. Our measurements confirm theoretical predictions, and support the picture that proximity to charge ordered states is a general property of superconductivity in copper oxides.     

Emergence of preformed Cooper pairs from the doped Mott insulating state in Bi2Sr2CaCu2O8+delta

Superconductors are characterized by an energy gap that represents the energy needed to break the pairs of electrons (Cooper pairs) apart. At temperatures considerably above those associated with superconductivity, the high-transition-temperature copper oxides have an additional 'pseudogap'. It has been unclear whether this represents preformed pairs of electrons that have not achieved the coherence necessary for superconductivity, or whether it reflects some alternative ground state that competes with superconductivity. Paired electrons should display particle-hole symmetry with respect to the Fermi level (the energy of the highest occupied level in the electronic system), but competing states need not show such symmetry. Here we report a photoemission study of the underdoped copper oxide Bi(2)Sr(2)CaCu(2)O(8+delta) that shows the opening of a symmetric gap only in the anti-nodal region, contrary to the expectation that pairing would take place in the nodal region. It is therefore evident that the pseudogap does reflect the formation of preformed pairs of electrons and that the pairing occurs only in well-defined directions of the underlying lattice.     

Unusual magnetic order in the pseudogap region of the superconductor HgBa2CuO4+delta

The pseudogap region of the phase diagram is an important unsolved puzzle in the field of high-transition-temperature (high-T(c)) superconductivity, characterized by anomalous physical properties. There are open questions about the number of distinct phases and the possible presence of a quantum-critical point underneath the superconducting dome. The picture has remained unclear because there has not been conclusive evidence for a new type of order. Neutron scattering measurements for YBa(2)Cu(3)O(6+delta) (YBCO) resulted in contradictory claims of no and weak magnetic order, and the interpretation of muon spin relaxation measurements on YBCO and of circularly polarized photoemission experiments on Bi(2)Sr(2)CaCu(2)O(8+delta)(refs 12, 13) has been controversial. Here we use polarized neutron diffraction to demonstrate for the model superconductor HgBa(2)CuO(4+delta) (Hg1201) that the characteristic temperature T* marks the onset of an unusual magnetic order. Together with recent results for YBCO, this observation constitutes a demonstration of the universal existence of such a state. The findings appear to rule out theories that regard T* as a crossover temperature rather than a phase transition temperature. Instead, they are consistent with a variant of previously proposed charge-current-loop order that involves apical oxygen orbitals, and with the notion that many of the unusual properties arise from the presence of a quantum-critical point.     

Phase transitions in the incoherent lattice fluctuations in YBa2Cu3O(7-delta)

The growing body of experimental evidence for the existence of complex textures of charges and spins in the high-temperature superconductors has drawn attention to the so-called 'stripe-phase' models as a possible basis for the mechanism of superconductivity in these materials. Such observations have until now been restricted to systems where the texture dynamics are slow or suppressed altogether, and do not include the important case of YBa2Cu3O(7-delta). It seems likely that the dynamic behaviour of stripes, which has been suggested to undergo several phase transitions as a function of temperature, should also be reflected in the lattice properties of the host materials, and this forms the motivation for our present experiments. Specifically, we use MeV helium ion channelling, an ultrafast real-space probe of atomic displacements (with sub-picometre resolution), to probe incoherent lattice fluctuations in YBa2Cu3O(7-delta) as a function of temperature and oxygen doping. We detect lattice fluctuations that are larger than the expected thermal vibration component, and which show anomalies characteristic of the phase transitions anticipated for a dynamic stripe phase. Comparison of our lattice results with single-particle-tunnelling and photoemission data highlights the importance of spin-charge separation phenomena in the copper oxide superconductors.     

Microscopic electronic inhomogeneity in the high-Tc superconductor Bi2Sr2CaCu2O8+x

The parent compounds of the copper oxide high-transition-temperature (high-Tc) superconductors are unusual insulators (so-called Mott insulators). Superconductivity arises when they are 'doped' away from stoichiometry. For the compound Bi2Sr2CaCu2O8+x, doping is achieved by adding extra oxygen atoms, which introduce positive charge carriers ('holes') into the CuO2 planes where the superconductivity is believed to originate. Aside from providing the charge carriers, the role of the oxygen dopants is not well understood, nor is it clear how the charge carriers are distributed on the planes. Many models of high-Tc superconductivity accordingly assume that the introduced carriers are distributed uniformly, leading to an electronically homogeneous system as in ordinary metals. Here we report the presence of an electronic inhomogeneity in Bi2Sr2CaCu2O8+x, on the basis of observations using scanning tunnelling microscopy and spectroscopy. The inhomogeneity is manifested as spatial variations in both the local density of states spectrum and the superconducting energy gap. These variations are correlated spatially and vary on the surprisingly short length scale of approximately 14 A. Our analysis suggests that this inhomogeneity is a consequence of proximity to a Mott insulator resulting in poor screening of the charge potentials associated with the oxygen ions left in the BiO plane after doping, and is indicative of the local nature of the superconducting state.