Charge Density Waves in YBa_{2}Cu_{3}O_{6.67} Probed by Resonant X-Ray Scattering under Uniaxial Compression.

We report a comprehensive Cu L_{3}-edge resonant x-ray scattering (RXS) study of two- and three-dimensional (2D and 3D) incommensurate charge correlations in single crystals of the underdoped high-temperature superconductor YBa_{2}Cu_{3}O_{6.67} under uniaxial compression up to 1% along the two inequivalent Cu─O─Cu bond directions (a and b) in the CuO_{2} planes. We confirm the strong in-plane anisotropy of the 2D charge correlations and observe their symmetric response to pressure: pressure along a enhances correlations along b, and vice versa. Our results imply that the underlying order parameter is uniaxial. In contrast, 3D long-range charge order is only observed along b in response to compression along a. Spectroscopic RXS measurements show that the 3D charge order resides exclusively in the CuO_{2} planes and may thus be generic to the cuprates. We discuss implications of these results for models of electronic nematicity and for the interplay between charge order and superconductivity.

Dynamical charge density fluctuations pervading the phase diagram of a Cu-based high-T c superconductor.

Charge density modulations have been observed in all families of high-critical temperature (T c) superconducting cuprates. Although they are consistently found in the underdoped region of the phase diagram and at relatively low temperatures, it is still unclear to what extent they influence the unusual properties of these systems. Using resonant x-ray scattering, we carefully determined the temperature dependence of charge density modulations in YBa2Cu3O7-δ and Nd1+ x Ba2- x Cu3O7-δ for several doping levels. We isolated short-range dynamical charge density fluctuations in addition to the previously known quasi-critical charge density waves. They persist up to well above the pseudogap temperature T*, are characterized by energies of a few milli-electron volts, and pervade a large area of the phase diagram.

Three-dimensional collective charge excitations in electron-doped copper oxide superconductors.

High-temperature copper oxide superconductors consist of stacked CuO2 planes, with electronic band structures and magnetic excitations that are primarily two-dimensional1,2, but with superconducting coherence that is three-dimensional. This dichotomy highlights the importance of out-of-plane charge dynamics, which has been found to be incoherent in the normal state3,4 within the limited range of momenta accessible by optics. Here we use resonant inelastic X-ray scattering to explore the charge dynamics across all three dimensions of the Brillouin zone. Polarization analysis of recently discovered collective excitations (modes) in electron-doped copper oxides5-7 reveals their charge origin, that is, without mixing with magnetic components5-7. The excitations disperse along both the in-plane and out-of-plane directions, revealing its three-dimensional nature. The periodicity of the out-of-plane dispersion corresponds to the distance between neighbouring CuO2 planes rather than to the crystallographic c-axis lattice constant, suggesting that the interplane Coulomb interaction is responsible for the coherent out-of-plane charge dynamics. The observed properties are hallmarks of the long-sought 'acoustic plasmon', which is a branch of distinct charge collective modes predicted for layered systems8-12 and argued to play a substantial part in mediating high-temperature superconductivity10-12.

Re-entrant charge order in overdoped (Bi,Pb)2.12Sr1.88CuO6+δ outside the pseudogap regime.

In the underdoped regime, the cuprate high-temperature superconductors exhibit a host of unusual collective phenomena, including unconventional spin and charge density modulations, Fermi surface reconstructions, and a pseudogap in various physical observables. Conversely, overdoped cuprates are generally regarded as conventional Fermi liquids possessing no collective electronic order. In partial contradiction to this widely held picture, we report resonant X-ray scattering measurements revealing incommensurate charge order reflections for overdoped (Bi,Pb)2.12Sr1.88CuO6+δ (Bi2201), with correlation lengths of 40-60 lattice units, that persist up to temperatures of at least 250 K. The value of the charge order wavevector decreases with doping, in line with the extrapolation of the trend previously observed in underdoped Bi2201. In overdoped materials, however, charge order coexists with a single, unreconstructed Fermi surface without nesting or pseudogap features. The discovery of re-entrant charge order in Bi2201 thus calls for investigations in other cuprate families and for a reconsideration of theories that posit an essential relationship between these phenomena.

High-temperature charge density wave correlations in La1.875Ba0.125CuO4 without spin-charge locking.

Although all superconducting cuprates display charge-ordering tendencies, their low-temperature properties are distinct, impeding efforts to understand the phenomena within a single conceptual framework. While some systems exhibit stripes of charge and spin, with a locked periodicity, others host charge density waves (CDWs) without any obviously related spin order. Here we use resonant inelastic X-ray scattering to follow the evolution of charge correlations in the canonical stripe-ordered cuprate La1.875Ba0.125CuO4 across its ordering transition. We find that high-temperature charge correlations are unlocked from the wavevector of the spin correlations, signaling analogies to CDW phases in various other cuprates. This indicates that stripe order at low temperatures is stabilized by the coupling of otherwise independent charge and spin density waves, with important implications for the relation between charge and spin correlations in the cuprates.

Crossover from Collective to Incoherent Spin Excitations in Superconducting Cuprates Probed by Detuned Resonant Inelastic X-Ray Scattering.

Spin excitations in the overdoped high temperature superconductors Tl_{2}Ba_{2}CuO_{6+δ} and (Bi,Pb)_{2}(Sr,La)_{2}CuO_{6+δ} were investigated by resonant inelastic x-ray scattering (RIXS) as functions of doping and detuning of the incoming photon energy above the Cu-L_{3} absorption peak. The RIXS spectra at optimal doping are dominated by a paramagnon feature with peak energy independent of photon energy, similar to prior results on underdoped cuprates. Beyond optimal doping, the RIXS data indicate a sharp crossover to a regime with a strong contribution from incoherent particle-hole excitations whose maximum shows a fluorescencelike shift upon detuning. The spectra of both compound families are closely similar, and their salient features are reproduced by exact-diagonalization calculations of the single-band Hubbard model on a finite cluster. The results are discussed in the light of recent transport experiments indicating a quantum phase transition near optimal doping.

RixsToolBox: software for the analysis of soft X-ray RIXS data acquired with 2D detectors.

A software with a graphical user interface has been developed with the aim of facilitating the data analysis for users of a new resonant inelastic X-ray scattering (RIXS) spectrometer installed at the ESRF beamline ID32. The software is organized in modules covering all relevant steps in the data reduction from a stack of several hundred two-dimensional CCD images to a single RIXS spectrum. It utilizes both full charge integration and single-photon centroiding to cope with high-flux and high-resolution requirements. Additional modules for further data analysis and the extraction of instrumental parameters are available. The software has been in routine use for about a year now and in that time many additional features have been incorporated. It now meets the users' need for an easy-to-use data analysis tool that allows looking at and understanding data as it is acquired and thus steering users' experiments more efficiently.

Collective nature of spin excitations in superconducting cuprates probed by resonant inelastic X-ray scattering.

We used resonant inelastic x-ray scattering (RIXS) with and without analysis of the scattered photon polarization, to study dispersive spin excitations in the high temperature superconductor YBa_{2}Cu_{3}O_{6+x} over a wide range of doping levels (0.1≤x≤1). The excitation profiles were carefully monitored as the incident photon energy was detuned from the resonant condition, and the spin excitation energy was found to be independent of detuning for all x. These findings demonstrate that the largest fraction of the spin-flip RIXS profiles in doped cuprates arises from magnetic collective modes, rather than from incoherent particle-hole excitations as recently suggested theoretically [Benjamin et al. Phys. Rev. Lett. 112, 247002 (2014)]. Implications for the theoretical description of the electron system in the cuprates are discussed.

Charge order and its connection with Fermi-liquid charge transport in a pristine high-T(c) cuprate.

Electronic inhomogeneity appears to be an inherent characteristic of the enigmatic cuprate superconductors. Here we report the observation of charge-density-wave correlations in the model cuprate superconductor HgBa2CuO(4+δ) (T(c)=72 K) via bulk Cu L3-edge-resonant X-ray scattering. At the measured hole-doping level, both the short-range charge modulations and Fermi-liquid transport appear below the same temperature of about 200 K. Our result points to a unifying picture in which these two phenomena are preceded at the higher pseudogap temperature by q=0 magnetic order and the build-up of significant dynamic antiferromagnetic correlations. The magnitude of the charge modulation wave vector is consistent with the size of the electron pocket implied by quantum oscillation and Hall effect measurements for HgBa2CuO(4+δ) and with corresponding results for YBa2Cu3O(6+δ), which indicates that charge-density-wave correlations are universally responsible for the low-temperature quantum oscillation phenomenon.

The simultaneous measurement of energy and linear polarization of the scattered radiation in resonant inelastic soft x-ray scattering.

Resonant Inelastic X-ray Scattering (RIXS) in the soft x-ray range is an element-specific energy-loss spectroscopy used to probe the electronic and magnetic excitations in strongly correlated solids. In the recent years, RIXS has been progressing very quickly in terms of energy resolution and understanding of the experimental results, but the interpretation of spectra could further improve, sometimes decisively, from a full knowledge of the polarization of incident and scattered photons. Here we present the first implementation, in a high resolution soft-RIXS spectrometer used to analyze the scattered radiation, of a device allowing the measurement of the degree of linear polarization. The system, based on a graded W/B4C multilayer mirror installed in proximity of the CCD detector, has been installed on the AXES spectrometer at the ESRF (European Synchrotron Radiation Facility); it has been fully characterized and it has been used for a demonstration experiment at the Cu L3 edge on a high-Tc superconducting cuprate. The loss in efficiency suffered by the spectrometer equipped with this test facility was a factor 17.5. We propose also a more advanced version, suitable for a routine use on the next generation of RIXS spectrometers and with an overall efficiency up to 10%.

High-energy spin and charge excitations in electron-doped copper oxide superconductors.

The evolution of electronic (spin and charge) excitations upon carrier doping is an extremely important issue in superconducting layered cuprates and the knowledge of its asymmetry between electron- and hole-dopings is still fragmentary. Here we combine X-ray and neutron inelastic scattering measurements to track the doping dependence of both spin and charge excitations in electron-doped materials. Copper L3 resonant inelastic X-ray scattering spectra show that magnetic excitations shift to higher energy upon doping. Their dispersion becomes steeper near the magnetic zone centre and they deeply mix with charge excitations, indicating that electrons acquire a highly itinerant character in the doped metallic state. Moreover, above the magnetic excitations, an additional dispersing feature is observed near the Γ-point, and we ascribe it to particle-hole charge excitations. These properties are in stark contrast with the more localized spin excitations (paramagnons) recently observed in hole-doped compounds even at high doping levels.

Opening of a Peierls gap in BaVS3 probed by V L3 edge resonant inelastic x-ray scattering.

V L3 edge resonant inelastic x-ray scattering measurements performed on high quality BaVS3 single crystals reveal that the intra-t2g dd excitations close to the elastic peak are suppressed below the metal-insulator transition induced by the Peierls instability. The depletion of electronic states close to the Fermi level represents a direct observation of the opening of a charge gap inside the t2g manifold.

Persistence of magnetic excitations in La(2-x)Sr(x)CuO4 from the undoped insulator to the heavily overdoped non-superconducting metal.

One of the most intensely studied scenarios of high-temperature superconductivity (HTS) postulates pairing by exchange of magnetic excitations. Indeed, such excitations have been observed up to optimal doping in the cuprates. In the heavily overdoped regime, neutron scattering measurements indicate that magnetic excitations have effectively disappeared, and this has been argued to cause the demise of HTS with overdoping. Here we use resonant inelastic X-ray scattering, which is sensitive to complementary parts of reciprocal space, to measure the evolution of the magnetic excitations in La(2-x)Sr(x)CuO4 across the entire phase diagram, from a strongly correlated insulator (x = 0) to a non-superconducting metal (x = 0.40). For x = 0, well-defined magnon excitations are observed. These magnons broaden with doping, but they persist with a similar dispersion and comparable intensity all the way to the non-superconducting, heavily overdoped metallic phase. The destruction of HTS with overdoping is therefore caused neither by the general disappearance nor by the overall softening of magnetic excitations. Other factors, such as the redistribution of spectral weight, must be considered.

Momentum-dependent charge correlations in YBa2Cu3O6+δ superconductors probed by resonant X-ray scattering: evidence for three competing phases.

We use resonant x-ray scattering to determine the momentum-dependent charge correlations in YBa(2)Cu(3) O(6.55) samples with highly ordered chain arrays of oxygen acceptors (ortho-II structure). The results reveal nearly critical, biaxial charge density wave (CDW) correlations at in-plane wave vectors (0.315, 0) and (0, 0.325). The corresponding scattering intensity exhibits a strong uniaxial anisotropy. The CDW amplitude and correlation length are enhanced as superconductivity is weakened by an external magnetic field. Analogous experiments are carried out on a YBa(2)Cu(3)O(6.6) crystal with a dilute concentration of spinless (Zn) impurities, which had earlier been shown to nucleate incommensurate magnetic order. Compared to pristine crystals with the same doping level, the CDW amplitude and correlation length are found to be strongly reduced. These results indicate a three-phase competition between spin-modulated, charge-modulated, and superconducting states in underdoped YBa(2)Cu(3)O(6+δ).

Distinct charge orders in the planes and chains of ortho-III-ordered YBa2Cu3O(6+δ) superconductors identified by resonant elastic x-ray scattering.

Recently, charge density wave (CDW) order in the CuO(2) planes of underdoped YBa(2)Cu(3)O(6+δ) was detected using resonant soft x-ray scattering. An important question remains: is the chain layer responsible for this charge ordering? Here, we explore the energy and polarization dependence of the resonant scattering intensity in a detwinned sample of YBa(2)Cu(3)O(6.75) with ortho-III oxygen ordering in the chain layer. We show that the ortho-III CDW order in the chains is distinct from the CDW order in the planes. The ortho-III structure gives rise to a commensurate superlattice reflection at Q=[0.33 0 L] whose energy and polarization dependence agrees with expectations for oxygen ordering and a spatial modulation of the Cu valence in the chains. Incommensurate peaks at [0.30 0 L] and [0 0.30 L] from the CDW order in the planes are shown to be distinct in Q as well as their temperature, energy, and polarization dependence, and are thus unrelated to the structure of the chain layer. Moreover, the energy dependence of the CDW order in the planes is shown to result from a spatial modulation of energies of the Cu 2p to 3d(x(2)-y(2)) transition, similar to stripe-ordered 214 cuprates.

Long-range incommensurate charge fluctuations in (Y,Nd)Ba2Cu3O(6+x).

The concept that superconductivity competes with other orders in cuprate superconductors has become increasingly apparent, but obtaining direct evidence with bulk-sensitive probes is challenging. We have used resonant soft x-ray scattering to identify two-dimensional charge fluctuations with an incommensurate periodicity of ~3.2 lattice units in the copper-oxide planes of the superconductors (Y,Nd)Ba(2)Cu(3)O(6+)(x), with hole concentrations of 0.09 to 0.13 per planar Cu ion. The intensity and correlation length of the fluctuation signal increase strongly upon cooling down to the superconducting transition temperature (T(c)); further cooling below T(c) abruptly reverses the divergence of the charge correlations. In combination with earlier observations of a large gap in the spin excitation spectrum, these data indicate an incipient charge density wave instability that competes with superconductivity.

BaVS3 probed by V L edge x-ray absorption spectroscopy.

Polarization dependent vanadium L edge x-ray absorption spectra of BaVS(3) single crystals are measured in the four phases of the compound. The difference between signals with the polarizations E perpendicular to c and E is parallel to c (linear dichroism) changes with temperature. Besides increasing the intensity of one of the maxima, a new structure appears in the pre-edge region below the metal-insulator transition. More careful examination brings to light that the changes start already with pretransitional charge density wave fluctuations. Simple symmetry analysis suggests that the effect is related to rearrangements in the E(g) and A(1g) states, and is compatible with the formation of four inequivalent V-sites along the V-S chain.

Magnetic excitations and phase separation in the underdoped La2-xSrxCuO4 superconductor measured by resonant inelastic X-ray scattering.

We probe the collective magnetic modes of La2CuO4 and underdoped La2-xSrxCuO4 (LSCO) by momentum resolved resonant inelastic x-ray scattering (RIXS) at the Cu L3 edge. For the undoped antiferromagnetic sample, we show that the single magnon dispersion measured with RIXS coincides with the one determined by inelastic neutron scattering, thus demonstrating that x rays are an alternative to neutrons in this field. In the spin dynamics of LSCO, we find a branch dispersing up to approximately 400 meV coexisting with one at lower energy. The high-energy branch has never been seen before. It indicates that underdoped LSCO is in a dynamic inhomogeneous spin state.

Measurement of magnetic excitations in the two-dimensional antiferromagnetic Sr2CuO2Cl2 insulator using resonant x-ray scattering: evidence for extended interactions.

We measured the momentum dependence of magnetic excitations in the model spin-1/2 2D antiferromagnetic insulator Sr2CuO2Cl2 (SCOC). We identify a single-spin-wave feature and a multimagnon continuum, with different polarization dependences. The spin waves display a large (70 meV) dispersion between the zone-boundary points (π, 0) and (π/2, π/2). Employing an extended t-t'-t''-U one-band Hubbard model, we find significant electronic hopping beyond nearest-neighbor Cu ions, indicative of extended magnetic interactions. The spectral line shape at (π, 0) indicates sizable quantum effects in SCOC and probably more generally in the cuprates.

Momentum dependence of orbital excitations in Mott-insulating titanates.

High-resolution resonant inelastic x-ray scattering has been used to determine the momentum dependence of orbital excitations in Mott-insulating LaTiO(3) and YTiO(3) over a wide range of the Brillouin zone. The data are compared to calculations in the framework of lattice-driven and superexchange-driven orbital ordering models. A superexchange model in which the experimentally observed modes are attributed to two-orbiton excitations yields the best description of the data.