Transition from a uni- to a bimodal interfacial charge distribution in [Formula: see text]/[Formula: see text] upon cooling.

We present a combined resonant soft X-ray reflectivity and electric transport study of [Formula: see text]/[Formula: see text] field effect devices. The depth profiles with atomic layer resolution that are obtained from the resonant reflectivity reveal a pronounced temperature dependence of the two-dimensional electron liquid at the [Formula: see text]/[Formula: see text] interface. At room temperature the corresponding electrons are located close to the interface, extending down to 4 unit cells into the [Formula: see text] substrate. Upon cooling, however, these interface electrons assume a bimodal depth distribution: They spread out deeper into the [Formula: see text] and split into two distinct parts, namely one close to the interface with a thickness of about 4 unit cells and another centered around 9 unit cells from the interface. The results are consistent with theoretical predictions based on oxygen vacancies at the surface of the [Formula: see text] film and support the notion of a complex interplay between structural and electronic degrees of freedom.

Site-selective spectroscopy with depth resolution using resonant x-ray reflectometry.

Combining dissimilar transition metal oxides (TMOs) into artificial heterostructures enables to create electronic interface systems with new electronic properties that do not exist in bulk. A detailed understanding of how such interfaces can be used to tailor physical properties requires characterization techniques capable to yield interface sensitive spectroscopic information with monolayer resolution. In this regard resonant x-ray reflectivity (RXR) provides a unique experimental tool to achieve exactly this. It yields the element specific electronic depth profiles in a non-destructive manner. Here, using a YBa2Cu3O7-δ (YBCO) thin film, we demonstrate that RXR is further capable to deliver site selectivity. By applying a new analysis scheme to RXR, which takes the atomic structure of the material into account, together with information of the local charge anisotropy of the resonant ions, we obtained spectroscopic information from the different Cu sites (e.g., chain and plane) throughout the film profile. While most of the film behaves bulk-like, we observe that the Cu-chains at the surface show characteristics of electron doping, whereas the Cu-planes closest to the surface exhibit an orbital reconstruction similar to that observed at La1-x Ca x MnO3/YBCO interfaces.

Nematicity in stripe-ordered cuprates probed via resonant x-ray scattering.

In underdoped cuprate superconductors, a rich competition occurs between superconductivity and charge density wave (CDW) order. Whether rotational symmetry-breaking (nematicity) occurs intrinsically and generically or as a consequence of other orders is under debate. Here, we employ resonant x-ray scattering in stripe-ordered superconductors (La,M)2CuO4 to probe the relationship between electronic nematicity of the Cu 3d orbitals, structure of the (La,M)2O2 layers, and CDW order. We find distinct temperature dependences for the structure of the (La,M)2O2 layers and the electronic nematicity of the CuO2 planes, with only the latter being enhanced by the onset of CDW order. These results identify electronic nematicity as an order parameter that is distinct from a purely structural order parameter in underdoped striped cuprates.

Orbital symmetry of charge-density-wave order in La1.875Ba0.125CuO4 and YBa2Cu3O6.67.

Recent theories of charge-density-wave (CDW) order in high-temperature superconductors have predicted a primarily d CDW orbital symmetry. Here, we report on the orbital symmetry of CDW order in the canonical cuprate superconductors La1.875Ba0.125CuO4 (LBCO) and YBa2Cu3O6.67 (YBCO), using resonant soft X-ray scattering and a model mapped to the CDW orbital symmetry. From measurements sensitive to the O sublattice, we conclude that LBCO has predominantly s' CDW orbital symmetry, in contrast to the d orbital symmetry recently reported in other cuprates. Furthermore, we show for YBCO that the CDW orbital symmetry differs along the a and b crystal axes and that these both differ from LBCO. This work highlights CDW orbital symmetry as an additional key property that distinguishes the different cuprate families. We discuss how the CDW symmetry may be related to the '1/8-anomaly' and to static spin ordering.

Observation of a Devil's Staircase in the Novel Spin-Valve System SrCo6O11.

Using resonant soft-x-ray scattering as a function of both temperature and magnetic field, we reveal a large number of almost degenerate magnetic orders in SrCo6O11. The Ising-like spins in this frustrated material in fact exhibit a so-called magnetic devil's staircase. It is demonstrated how a magnetic field induces transitions between different microscopic spin configurations, which is responsible for the magnetoresistance of SrCo6O11. This material therefore constitutes a unique combination of a magnetic devil's staircase and spin-valve effects, yielding a novel type of magnetoresistance system.

Magnetic moments and exchange coupling in nitride clusterfullerenes Gd(x)Sc(3-x)N@C80 (x = 1-3).

The magnetic properties of nitride clusterfullerenes GdxSc3-xN@C80 (x = 1-3) are studied as a function of the number of Gd atoms in the cluster. The intracluster interaction of the Gd ions in Gd2ScN@C80 and Gd3N@C80 is ferromagnetic with exchange constants of -1.2 K ± 0.1 K and -0.6 K ± 0.1 K, respectively. At 2 K, the magnetization curves exhibit noticeable deviations from the Heisenberg model pointing to a non-negligible anisotropy.

Electronic superlattice revealed by resonant scattering from random impurities in Sr3Ru2O7.

Resonant elastic x-ray scattering (REXS) is an exquisite element-sensitive tool for the study of subtle charge, orbital, and spin superlattice orders driven by the valence electrons, which therefore escape detection in conventional x-ray diffraction (XRD). Although the power of REXS has been demonstrated by numerous studies of complex oxides performed in the soft x-ray regime, the cross section and photon wavelength of the material-specific elemental absorption edges ultimately set the limit to the smallest superlattice amplitude and periodicity one can probe. Here we show--with simulations and REXS on Mn-substituted Sr3Ru2O7--that these limitations can be overcome by performing resonant scattering experiments at the absorption edge of a suitably-chosen, dilute impurity. This establishes that--in analogy with impurity-based methods used in electron-spin-resonance, nuclear-magnetic resonance, and Mössbauer spectroscopy--randomly distributed impurities can serve as a non-invasive, but now momentum-dependent probe, greatly extending the applicability of resonant x-ray scattering techniques.

Resonant elastic soft x-ray scattering.

Resonant (elastic) soft x-ray scattering (RSXS) offers a unique element, site and valence specific probe to study spatial modulations of charge, spin and orbital degrees of freedom in solids on the nanoscopic length scale. It is not only used to investigate single-crystalline materials. This method also enables one to examine electronic ordering phenomena in thin films and to zoom into electronic properties emerging at buried interfaces in artificial heterostructures. During the last 20 years, this technique, which combines x-ray scattering with x-ray absorption spectroscopy, has developed into a powerful probe to study electronic ordering phenomena in complex materials and furthermore delivers important information on the electronic structure of condensed matter. This review provides an introduction to the technique, covers the progress in experimental equipment, and gives a survey on recent RSXS studies of ordering in correlated electron systems and at interfaces.

Resonant X-ray scattering measurements of a spatial modulation of the Cu 3d and O 2p energies in stripe-ordered cuprate superconductors.

A prevailing description of the stripe phase in underdoped cuprate superconductors is that the charge carriers (holes) phase segregate on a microscopic scale into hole-rich and hole-poor regions. We report resonant elastic x-ray scattering measurements of stripe-ordered La(1.475)Nd(0.4)Sr(0.125)CuO(4) at the Cu L and O K absorption edges that identify an additional feature of stripe order. Analysis of the energy dependence of the scattering intensity reveals that the dominant signature of the stripe order is a spatial modulation in the energies of Cu 3d and O 2p states rather than the large modulation of the charge density (valence) envisioned in the common stripe paradigm. These energy shifts are interpreted as a spatial modulation of the electronic structure and may point to a valence-bond-solid interpretation of the stripe phase.

Probing the role of co substitution in the electronic structure of iron pnictides.

The role of Co substitution in the low-energy electronic structure of Ca(Fe(0.944)Co(0.056))(2)As(2) is investigated by resonant photoemission spectroscopy and density-functional theory. The Co 3d state center of mass is observed at 250 meV higher binding energy than that of Fe, indicating that Co possesses one extra valence electron and that Fe and Co are in the same oxidation state. Yet, significant Co character is detected for the Bloch wave functions at the chemical potential, revealing that the Co 3d electrons are part of the Fermi sea determining the Fermi surface. This establishes the complex role of Co substitution in CaFe(2)As(2) and the inadequacy of a rigid-band shift description.

Electronic confinement and ordering instabilities in colossal magnetoresistive bilayer manganites.

We present angle-resolved photoemission studies of (La{1-z}Pr{z}){2-2x}Sr{1+2x}Mn{2}O{7} with x=0.4 and z=0.1, 0.2, and 0.4 along with density functional theory calculations and x-ray scattering data. Our results show that the bilayer splitting in the ferromagnetic metallic phase of these materials is small, if not completely absent. The charge carriers are therefore confined to a single MnO{2} layer, which in turn results in a strongly nested Fermi surface. In addition to this, the spectral function also displays clear signatures of an electronic ordering instability well below the Fermi level. The increase of the corresponding interaction strength with z and its magnitude of ∼400 meV make the coupling to a bare phonon highly unlikely. Instead we conclude that fluctuating order, involving electronic and lattice degrees of freedom, causes the observed renormalization of the spectral features.

Magnetic frustration, phase competition, and the magnetoelectric effect in NdFe3(BO3)4.

We present an element selective resonant magnetic x-ray scattering study of NdFe3(BO3)4 as a function of temperature and applied magnetic field. Our measurements show that the magnetic order of the Nd sublattice is induced by the Fe spin order. When a magnetic field is applied parallel to the hexagonal basal plane, the helicoidal spin order is suppressed and a collinear ordering, where the moments are forced to align in a direction perpendicular to the applied magnetic field, is stabilized. This result excludes a noncollinear spin order as the origin of the magnetically induced electric polarization in this compound. Instead our data imply that magnetic frustration results in a phase competition, which is the origin of the magnetoelectric response.

An in-vacuum diffractometer for resonant elastic soft x-ray scattering.

We describe the design, construction, and performance of a 4-circle in-vacuum diffractometer for resonant elastic soft x-ray scattering. The diffractometer, installed on the resonant elastic and inelastic x-ray scattering beamline at the Canadian Light Source, includes 9 in-vacuum motions driven by in-vacuum stepper motors and operates in ultra-high vacuum at base pressure of 2 × 10(-10) Torr. Cooling to a base temperature of 18 K is provided with a closed-cycle cryostat. The diffractometer includes a choice of 3 photon detectors: a photodiode, a channeltron, and a 2D sensitive channelplate detector. Along with variable slit and filter options, these detectors are suitable for studying a wide range of phenomena having both weak and strong diffraction signals. Example measurements of diffraction and reflectivity in Nd-doped (La,Sr)(2)CuO(4) and thin film (Ga,Mn)As are shown.

Observation of electronic ferroelectric polarization in multiferroic YMn2O5.

We report the observation of a magnetic polarization of the O 2p states in YMn(2)O(5) through the use of soft x-ray resonant scattering at the oxygen K edge. Remarkably, we find that the temperature dependence of the integrated intensity of this signal closely follows the macroscopic electric polarization, and hence is proportional to the ferroelectric order parameter. This is in contrast with the temperature dependence observed at the Mn L(3) edge, which reflects the Mn magnetic order parameter. First-principles calculations provide a microscopic understanding of these results and show that a spin-dependent hybridization of O 2p and Mn 3d states results in a purely electronic contribution to the ferroelectric polarization, which can exist in the absence of lattice distortions.

Anomalous quasiparticle renormalization in Na0.73CoO2: role of interorbital interactions and magnetic correlations.

We report an angular resolved photoemission study of NaxCoO2 with x approximately 0.73 where it is found that the renormalization of the quasiparticle (QP) dispersion changes dramatically upon a rotation from GammaM to GammaK. The comparison of the experimental data to the calculated band structure reveals that the quasiparticle renormalization is most pronounced along the GammaK direction, while it is significantly weaker along the GammaM direction. We discuss the observed anisotropy in terms of multiorbital effects and point out the relevance of magnetic correlations for the band structure of NaxCoO2 with x approximately 0.75.

Stripe correlations in Na(0.75)CoO2.

We present a combined high-energy x-ray diffraction and local-density approximation study of the sodium ordering in Na(0.75)CoO2. The obtained results rule out previously proposed Na-ordering models and provide strong evidence for the formation of sodium-density stripes in this material. The local-density approximation calculations prove that the sodium-density stripes lead to a sizable dip in the density of the Co states at the Fermi level, pointing to band structure effects as a driving force for the stripe formation. This indicates that the sodium ordering is connected to stripelike charge correlations within the CoO2 layers, leading to an astonishing similarity between the doped cuprates and the NaxCoO2 compounds.

Constituents of the quasiparticle spectrum along the nodal direction of high-Tc cuprates.

Applying the Kramers-Kronig consistent procedure, developed earlier, we investigate in detail the formation of the quasiparticle spectrum along the nodal direction of high-Tc cuprates. The heavily discussed "70 meV kink" on the renormalized dispersion exhibits a strong temperature and doping dependence when purified from structural effects such as bilayer splitting, diffraction replicas, etc. This dependence is well understood in terms of fermionic and bosonic constituents of the self-energy. The latter follows the evolution of the spin-fluctuation spectrum, emerging below some doping dependent temperature and sharpening below Tc, and is mainly responsible for the formation of the kink in question.

Kinks, nodal bilayer splitting, and interband scattering in YBa2Cu3O(6+x).

We apply the new-generation angle-resolved photoemission spectroscopy methodology to the most widely studied cuprate superconductor YBa2Cu3O(6+x). Considering the nodal direction, we found noticeable renormalization effects known as kinks both in the quasiparticle dispersion and scattering rate, the bilayer splitting, and evidence for strong interband scattering--all the characteristic features of the nodal quasiparticles detected earlier in Bi2Sr2CaCu2O(8+delta). The typical energy scale and the doping dependence of the kinks clearly point to their intimate relation with the spin-1 resonance seen in the neutron scattering experiments. Our findings strongly suggest a universality of the electron dynamics in the bilayer superconducting cuprates and a dominating role of the spin fluctuations in the formation of the quasiparticles along the nodal direction.

Parity of the pairing bosons in a high-temperature Pb-Bi2Sr2CaCu2O8 bilayer superconductor by angle-resolved photoemission spectroscopy.

We report the observation of a novel effect in the bilayer Pb-Bi2Sr2CaCu2O8 (Pb-Bi2212) high-T(c) superconductor by means of angle-resolved photoemission with circularly polarized excitation. Different scattering rates, determined as a function of energy separately for the bonding and antibonding copper-oxygen bands, strongly imply that the dominating scattering channel is odd with respect to layer exchange within a bilayer. This is inconsistent with a phonon-mediated scattering and favors the participation of the odd collective spin excitations in the scattering mechanism in near-nodal regions of the k space, suggesting a magnetic nature of the pairing mediator.

Effect of Zn and Ni impurities on the quasiparticle renormalization of superconducting Bi-2212.

The Cu substitution by Zn and Ni impurities and its influence on the mass renormalization effects in angle-resolved photoelectron spectra (ARPES) of Bi2Sr2CaCu2O8-delta is addressed. We show that the nonmagnetic Zn atoms have a much stronger effect in both the nodal and antinodal parts of the Brillouin zone than magnetic Ni. The observed changes are consistent with the behavior of the spin resonance mode as seen by inelastic neutron scattering in YBCO. This strongly suggests that the "peak-dip-hump" and the kink in ARPES on the one side and neutron resonance on the other are closely related features.