Spin correlations in the electron-doped high-transition-temperature superconductor Nd2-xCexCuO4+/-delta

High-transition-temperature (high-T(c)) superconductivity develops near antiferromagnetic phases, and it is possible that magnetic excitations contribute to the superconducting pairing mechanism. To assess the role of antiferromagnetism, it is essential to understand the doping and temperature dependence of the two-dimensional antiferromagnetic spin correlations. The phase diagram is asymmetric with respect to electron and hole doping, and for the comparatively less-studied electron-doped materials, the antiferromagnetic phase extends much further with doping and appears to overlap with the superconducting phase. The archetypal electron-doped compound Nd2-xCexCuO4+/-delta (NCCO) shows bulk superconductivity above x approximately 0.13 (refs 3, 4), while evidence for antiferromagnetic order has been found up to x approximately 0.17 (refs 2, 5, 6). Here we report inelastic magnetic neutron-scattering measurements that point to the distinct possibility that genuine long-range antiferromagnetism and superconductivity do not coexist. The data reveal a magnetic quantum critical point where superconductivity first appears, consistent with an exotic quantum phase transition between the two phases. We also demonstrate that the pseudogap phenomenon in the electron-doped materials, which is associated with pronounced charge anomalies, arises from a build-up of spin correlations, in agreement with recent theoretical proposals.     

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.     

Fluctuating stripes at the onset of the pseudogap in the high-T(c) superconductor Bi(2)Sr(2)CaCu(2)O(8+x)

Doped Mott insulators have a strong propensity to form patterns of holes and spins often referred to as stripes. In copper oxides, doping also gives rise to the pseudogap state, which can be transformed into a high-temperature superconducting state with sufficient doping or by reducing the temperature. A long-standing issue has been the interplay between the pseudogap, which is generic to all hole-doped copper oxide superconductors, and stripes, whose static form occurs in only one family of copper oxides over a narrow range of the phase diagram. Here we report observations of the spatial reorganization of electronic states with the onset of the pseudogap state in the high-temperature superconductor Bi(2)Sr(2)CaCu(2)O(8+x), using spectroscopic mapping with a scanning tunnelling microscope. We find that the onset of the pseudogap phase coincides with the appearance of electronic patterns that have the predicted characteristics of fluctuating stripes. As expected, the stripe patterns are strongest when the hole concentration in the CuO(2) planes is close to 1/8 (per copper atom). Although they demonstrate that the fluctuating stripes emerge with the onset of the pseudogap state and occur over a large part of the phase diagram, our experiments indicate that the stripes are a consequence of pseudogap behaviour rather than its cause.     

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.     

Coupling strength of charge carriers to spin fluctuations in high-temperature superconductors

In conventional superconductors, the most direct evidence of the mechanism responsible for superconductivity comes from tunnelling experiments, which provide a clear picture of the underlying electron-phonon interactions. As the coherence length in conventional superconductors is large, the tunnelling process probes several atomic layers into the bulk of the material; the observed structure in the current-voltage characteristics at the phonon energies gives, through inversion of the Eliashberg equations, the electron-phonon spectral density alpha2F(omega). The situation is different for the high-temperature copper oxide superconductors, where the coherence length (particularly for c-axis tunnelling) can be very short. Because of this, methods such as optical spectroscopy and neutron scattering provide a better route for investigating the underlying mechanism, as they probe bulk properties. Accurate reflection measurements at infrared wavelengths and precise polarized neutron-scattering data are now available for a variety of the copper oxides, and here we show that the conducting carriers (probed by infrared spectroscopy) are strongly coupled to a resonance structure in the spectrum of spin fluctuations (measured by neutron scattering). The coupling strength inferred from those results is sufficient to account for the high transition temperatures of the copper oxides, highlighting a prominent role for spin fluctuations in driving superconductivity in these materials.     

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.     

Vortex-like excitations and the onset of superconducting phase fluctuation in underdoped La(2-x)Sr(x)CuO4

Two general features of a superconductor, which appear at the critical temperature, are the formation of an energy gap and the expulsion of magnetic flux (the Meissner effect). In underdoped copper oxides, there is strong evidence that an energy gap (the pseudogap) opens up at a temperature significantly higher than the critical temperature (by 100-220 K). Certain features of the pseudogap suggest that it is closely related to the gap that appears at the critical temperature (for example, the variation of the gap magnitudes around the Fermi surface and their maximum amplitudes are very similar). However, the Meissner effect is absent in the pseudogap state. The nature of the pseudogap state, and its relation (if any) to the superconducting state are central issues in understanding copper oxide superconductivity. Recent evidence suggests that, in the underdoped regime, the Meissner state is destroyed above the critical temperature by strong phase fluctuations (as opposed to a vanishing of the superfluid density). Here we report evidence for vortices (or vortex-like excitations) in La(2-x)Sr(x)CuO4 at temperatures significantly above the critical temperature. A thermal gradient is applied to the sample in a magnetic field. Vortices are detected by the large transverse electric field produced as they diffuse down the gradient (the Nernst effect). We find that the Nernst signal is anomalously enhanced at temperatures as high as 150 K.     

Small phonon contribution to the photoemission kink in the copper oxide superconductors

Despite over two decades of intense research efforts, the origin of high-temperature superconductivity in the copper oxides remains elusive. Angle-resolved photoemission spectroscopy experiments have revealed a kink in the dispersion relations (energy versus wavevector) of electronic states in the copper oxides at binding energies of 50-80 meV, raising the hope that this anomaly could be a key to understanding high-temperature superconductivity. The kink is often interpreted in terms of interactions between the electrons and a bosonic field. Although there is no consensus on the nature of the bosons (or even whether a boson model is appropriate), both phonons and spin fluctuations have been proposed as possible candidates. Here we report first-principles calculations of the role of phonons and the electron-phonon interaction in the photoemission spectra of La(2 - x)Sr(x)CuO4. Our calculations within the standard formalism demonstrate that the phonon-induced renormalization of the electron energies and the Fermi velocity is almost one order of magnitude smaller than the effect observed in photoemission experiments. Therefore, our result rules out electron-phonon interaction in bulk La(2 - x)Sr(x)CuO4 as the exclusive origin of the measured kink. Our conclusions are consistent with those reached independently in a recent study of the related compound YBa2Cu3O7.     

Superconductor-insulator transition in La2 - xSrxCuO4 at the pair quantum resistance

High-temperature superconductivity in copper oxides arises when a parent insulator compound is doped beyond some critical concentration; what exactly happens at this superconductor-insulator transition is a key open question. The cleanest approach is to tune the carrier density using the electric field effect; for example, it was learned in this way that weak electron localization transforms superconducting SrTiO(3) into a Fermi-glass insulator. But in the copper oxides this has been a long-standing technical challenge, because perfect ultrathin films and huge local fields (>10(9)?V?m(-1)) are needed. Recently, such fields have been obtained using electrolytes or ionic liquids in the electric double-layer transistor configuration. Here we report synthesis of epitaxial films of La(2-?x)Sr(x)CuO(4) that are one unit cell thick, and fabrication of double-layer transistors. Very large fields and induced changes in surface carrier density enable shifts in the critical temperature by up to 30?K. Hundreds of resistance versus temperature and carrier density curves were recorded and shown to collapse onto a single function, as predicted for a two-dimensional superconductor-insulator transition. The observed critical resistance is precisely the quantum resistance for pairs, R(Q) = h/(2e) = 6.45?kΩ, suggestive of a phase transition driven by quantum phase fluctuations, and Cooper pair (de)localization.     

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.     

Nodal quasiparticle in pseudogapped colossal magnetoresistive manganites

A characteristic feature of the copper oxide high-temperature superconductors is the dichotomy between the electronic excitations along the nodal (diagonal) and antinodal (parallel to the Cu-O bonds) directions in momentum space, generally assumed to be linked to the 'd-wave' symmetry of the superconducting state. Angle-resolved photoemission measurements in the superconducting state have revealed a quasiparticle spectrum with a d-wave gap structure that exhibits a maximum along the antinodal direction and vanishes along the nodal direction. Subsequent measurements have shown that, at low doping levels, this gap structure persists even in the high-temperature metallic state, although the nodal points of the superconducting state spread out in finite 'Fermi arcs'. This is the so-called pseudogap phase, and it has been assumed that it is closely linked to the superconducting state, either by assigning it to fluctuating superconductivity or by invoking orders which are natural competitors of d-wave superconductors. Here we report experimental evidence that a very similar pseudogap state with a nodal-antinodal dichotomous character exists in a system that is markedly different from a superconductor: the ferromagnetic metallic groundstate of the colossal magnetoresistive bilayer manganite La1.2Sr1.8Mn2O7. Our findings therefore cast doubt on the assumption that the pseudogap state in the copper oxides and the nodal-antinodal dichotomy are hallmarks of the superconductivity state.     

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.     

电-声机制致高温超导特性随掺杂量演变

利用极性晶体中慢电子的运动规律提出基于BCS机理的分析模型.分析发现,掺杂导致铜氧化物的费米面电子分为低能费米电子和高能电子,并产生快电子效应.欠掺杂区高能电子与晶格振动发生作用形成赝隙,费米电子与晶格作用形成超导隙.赝隙和超导隙的竞争平衡导致欠掺杂区超导隙2Δ0和κBTc比值与高能费米电子速度vF^＊成正比,与费米速度vF成反比.掺杂量（x）与高能费米速度（vF^＊）相图是解释高温超导相图的基础.利用模型和（x-vF^＊）相图能够对欠掺杂区赝隙温度、能隙与κBTc比例随掺杂量增加而线性下降的现象给出简单解释,即最佳掺杂区2Δ0和κBTc比值为7.6、过掺杂区为4.3的常数.显示系统随掺杂量增加由＂非传统＂行为向接近传统行为再到金属行为演变的规律.     

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.     

Unconventional superconductivity in PuCoGa5

In the Bardeen-Cooper-Schrieffer theory of superconductivity, electrons form (Cooper) pairs through an interaction mediated by vibrations in the underlying crystal structure. Like lattice vibrations, antiferromagnetic fluctuations can also produce an attractive interaction creating Cooper pairs, though with spin and angular momentum properties different from those of conventional superconductors. Such interactions have been implicated for two disparate classes of materials--the copper oxides and a set of Ce- and U-based compounds. But because their transition temperatures differ by nearly two orders of magnitude, this raises the question of whether a common pairing mechanism applies. PuCoGa5 has a transition temperature intermediate between those classes and therefore may bridge these extremes. Here we report measurements of the nuclear spin-lattice relaxation rate and Knight shift in PuCoGa5, which demonstrate that it is an unconventional superconductor with properties as expected for antiferromagnetically mediated superconductivity. Scaling of the relaxation rates among all of these materials (a feature not exhibited by their Knight shifts) establishes antiferromagnetic fluctuations as a likely mechanism for their unconventional superconductivity and suggests that related classes of exotic superconductors may yet be discovered.     

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.     

A 'checkerboard' electronic crystal state in lightly hole-doped Ca2-xNaxCuO2Cl2

The phase diagram of hole-doped copper oxides shows four different electronic phases existing at zero temperature. Familiar among these are the Mott insulator, high-transition-temperature superconductor and metallic phases. A fourth phase, of unknown identity, occurs at light doping along the zero-temperature bound of the 'pseudogap' regime. This regime is rich in peculiar electronic phenomena, prompting numerous proposals that it contains some form of hidden electronic order. Here we present low-temperature electronic structure imaging studies of a lightly hole-doped copper oxide: Ca2-xNaxCuO2Cl2. Tunnelling spectroscopy (at energies |E| > 100 meV) reveals electron extraction probabilities greatly exceeding those for injection, as anticipated for a doped Mott insulator. However, for |E| < 100 meV, the spectrum exhibits a V-shaped energy gap centred on E = 0. States within this gap undergo intense spatial modulations, with the spatial correlations of a four CuO2-unit-cell square 'checkerboard', independent of energy. Intricate atomic-scale electronic structure variations also exist within the checkerboard. These data are consistent with an unanticipated crystalline electronic state, possibly the hidden electronic order, existing in the zero-temperature pseudogap regime of Ca2-xNaxCuO2Cl2.     

Superconductivity phase diagram of Na(x)CoO2*1.3H2O

The microscopic origin of superconductivity in the high-transition-temperature (high-T(c)) copper oxides remains the subject of active inquiry; several of their electronic characteristics are well established as universal to all the known materials, forming the experimental foundation that all theories must address. The most fundamental of those characteristics, for both the copper oxides and other superconductors, is the dependence of the superconducting T(c) on the degree of electronic band filling. The recent report of superconductivity near 4 K in the layered sodium cobalt oxyhydrate, Na(0.35)CoO2*1.3H2O, is of interest owing to both its triangular cobalt-oxygen lattice and its generally analogous chemical and structural relationships to the copper oxide superconductors. Here we show that the superconducting T(c) of this compound displays the same kind of behaviour on chemical doping that is observed in the high-T(c) copper oxides. Specifically, the optimal superconducting T(c) occurs in a narrow range of sodium concentrations (and therefore electron concentrations) and decreases for both underdoped and overdoped materials, as observed in the phase diagram of the copper oxide superconductors. The analogy is not perfect, however, suggesting that Na(x)CoO2*1.3H2O, with its triangular lattice geometry and special magnetic characteristics, may provide insights into systems where coupled charge and spin dynamics play an essential role in leading to superconductivity.     

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.     

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.