Charge and Spin Order Dichotomy in NdNiO_{2} Driven by the Capping Layer.

Superconductivity in infinite-layer nickelates holds exciting analogies with that of cuprates, with similar structures and 3d-electron count. Using resonant inelastic x-ray scattering, we studied electronic and magnetic excitations and charge density correlations in Nd_{1-x}Sr_{x}NiO_{2} thin films with and without an SrTiO_{3} capping layer. We observe dispersing magnons only in the capped samples, progressively dampened at higher doping. We detect an elastic resonant scattering peak in the uncapped x=0 compound at wave vector (∼⅓,0), remindful of the charge order signal in hole doped cuprates. The peak weakens at x=0.05 and disappears in the superconducting x=0.20 film. The role of the capping on the electronic reconstruction far from the interface remains to be understood.

A high-energy-resolution resonant inelastic X-ray scattering spectrometer at ID20 of the European Synchrotron Radiation Facility.

An end-station for resonant inelastic X-ray scattering and (resonant) X-ray emission spectroscopy at beamline ID20 of ESRF - The European Synchrotron is presented. The spectrometer hosts five crystal analysers in Rowland geometry for large solid angle collection and is mounted on a rotatable arm for scattering in both the horizontal and vertical planes. The spectrometer is optimized for high-energy-resolution applications, including partial fluorescence yield or high-energy-resolution fluorescence detected X-ray absorption spectroscopy and the study of elementary electronic excitations in solids. In addition, it can be used for non-resonant inelastic X-ray scattering measurements of valence electron excitations.

Direct tomography imaging for inelastic X-ray scattering experiments at high pressure.

A method to separate the non-resonant inelastic X-ray scattering signal of a micro-metric sample contained inside a diamond anvil cell (DAC) from the signal originating from the high-pressure sample environment is described. Especially for high-pressure experiments, the parasitic signal originating from the diamond anvils, the gasket and/or the pressure medium can easily obscure the sample signal or even render the experiment impossible. Another severe complication for high-pressure non-resonant inelastic X-ray measurements, such as X-ray Raman scattering spectroscopy, can be the proximity of the desired sample edge energy to an absorption edge energy of elements constituting the DAC. It is shown that recording the scattered signal in a spatially resolved manner allows these problems to be overcome by separating the sample signal from the spurious scattering of the DAC without constraints on the solid angle of detection. Furthermore, simple machine learning algorithms facilitate finding the corresponding detector pixels that record the sample signal. The outlined experimental technique and data analysis approach are demonstrated by presenting spectra of the Si L2,3-edge and O K-edge of compressed α-quartz. The spectra are of unprecedented quality and both the O K-edge and the Si L2,3-edge clearly show the existence of a pressure-induced phase transition between 10 and 24 GPa.

A large-solid-angle X-ray Raman scattering spectrometer at ID20 of the European Synchrotron Radiation Facility.

An end-station for X-ray Raman scattering spectroscopy at beamline ID20 of the European Synchrotron Radiation Facility is described. This end-station is dedicated to the study of shallow core electronic excitations using non-resonant inelastic X-ray scattering. The spectrometer has 72 spherically bent analyzer crystals arranged in six modular groups of 12 analyzer crystals each for a combined maximum flexibility and large solid angle of detection. Each of the six analyzer modules houses one pixelated area detector allowing for X-ray Raman scattering based imaging and efficient separation of the desired signal from the sample and spurious scattering from the often used complicated sample environments. This new end-station provides an unprecedented instrument for X-ray Raman scattering, which is a spectroscopic tool of great interest for the study of low-energy X-ray absorption spectra in materials under in situ conditions, such as in operando batteries and fuel cells, in situ catalytic reactions, and extreme pressure and temperature conditions.

Parametric Down-Conversion of X Rays into the Optical Regime.

We report the observation of parametrically down-converted x-ray signal photons at photon energies that correspond to idler photons at optical wavelengths. The count-rate dependence on the angles of the input beam and of the detector and on the slit sizes agrees with theory within the experimental uncertainties. The nonlinear susceptibility, which we calculated from the measured efficiencies, is comparable to the nonlinear susceptibility evaluated from the measurements of x-ray and optical wave mixing. The results of the present Letter advance the development of a spectroscopy method for probing valence-electron charges and the microscopic optical response of crystals with atomic-scale resolution.

Doping Evolution of Magnetic Order and Magnetic Excitations in (Sr_{1-x}La_{x})_{3}Ir_{2}O_{7}.

We use resonant elastic and inelastic x-ray scattering at the Ir-L_{3} edge to study the doping-dependent magnetic order, magnetic excitations, and spin-orbit excitons in the electron-doped bilayer iridate (Sr_{1-x}La_{x})_{3}Ir_{2}O_{7} (0≤x≤0.065). With increasing doping x, the three-dimensional long range antiferromagnetic order is gradually suppressed and evolves into a three-dimensional short range order across the insulator-to-metal transition from x=0 to 0.05, followed by a transition to two-dimensional short range order between x=0.05 and 0.065. Because of the interactions between the J_{eff}=1/2 pseudospins and the emergent itinerant electrons, magnetic excitations undergo damping, anisotropic softening, and gap collapse, accompanied by weakly doping-dependent spin-orbit excitons. Therefore, we conclude that electron doping suppresses the magnetic anisotropy and interlayer couplings and drives (Sr_{1-x}La_{x})_{3}Ir_{2}O_{7} into a correlated metallic state with two-dimensional short range antiferromagnetic order. Strong antiferromagnetic fluctuations of the J_{eff}=1/2 moments persist deep in this correlated metallic state, with the magnon gap strongly suppressed.

Persistent Paramagnons Deep in the Metallic Phase of Sr_{2-x}La_{x}IrO_{4}.

We have studied the magnetic excitations of electron-doped Sr_{2-x}La_{x}IrO_{4} (0≤x≤0.10) using resonant inelastic x-ray scattering at the Ir L_{3} edge. The long-range magnetic order is rapidly lost with increasing x, but two-dimensional short-range order (SRO) and dispersive magnon excitations with nearly undiminished spectral weight persist well into the metallic part of the phase diagram. The magnons in the SRO phase are heavily damped and exhibit anisotropic softening. Their dispersions are well described by a pseudospin-1/2 Heisenberg model with exchange interactions whose spatial range increases with doping. We also find a doping-independent high-energy magnetic continuum, which is not described by this model. The spin-orbit excitons arising from the pseudospin-3/2 manifold of the Ir ions broaden substantially in the SRO phase, but remain largely separated from the low-energy magnons. Pseudospin-1/2 models are therefore a good starting point for the theoretical description of the low-energy magnetic dynamics of doped iridates.

Resonant x-ray scattering and the j(eff) = 1/2 electronic ground state in iridate perovskites.

The resonant x-ray scattering (magnetic elastic, RXMS, and inelastic, RIXS) of Ir4+ at the L2,3 edges relevant to spin-orbit Mott insulators A(n+1)Ir(n)O(3n+1) (A = Sr, Ba, etc.) are calculated using a single-ion model which treats the spin-orbit and tetragonal crystal-field terms on an equal footing. Both RXMS and RIXS in the spin-flip channel are found to display a nontrivial dependence on the direction of the magnetic moment, µ. Crucially, we show that for µ in the ab plane, RXMS in the cross-polarized channel at the L2 edge is zero irrespective of the tetragonal crystal field; spin-flip RIXS, relevant to measurements of magnons, behaves reciprocally, being zero at L2 when µ is perpendicular to the ab plane. Our results have important implications for the assignment of a j(eff) = 1/2 ground state on the basis of resonant x-ray experiments.

Structural changes in amorphous Ge(x)SiO(y) on the way to nanocrystal formation.

Temperature induced changes of the local chemical structure of bulk amorphous GexSiOy are studied by Ge K-edge x-ray absorption near-edge spectroscopy and Si L2/3-edge x-ray Raman scattering spectroscopy. Different processes are revealed which lead to formation of Ge regions embedded in a Si oxide matrix due to different initial structures of as-prepared samples, depending on their Ge/Si/O ratio and temperature treatment, eventually resulting in the occurrence of nanocrystals. Here, disproportionation of GeOx and SiOx regions and/or reduction of Ge oxides by pure Si or by a surrounding Si sub-oxide matrix can be employed to tune the size of Ge nanocrystals along with the chemical composition of the embedding matrix. This is important for the optimization of the electronic and luminescent properties of the material.

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.

Resonant inelastic x-ray incarnation of Young's double-slit experiment.

Young's archetypal double-slit experiment forms the basis for modern diffraction techniques: The elastic scattering of waves yields an interference pattern that captures the real-space structure. Here, we report on an inelastic incarnation of Young's experiment and demonstrate that resonant inelastic x-ray scattering (RIXS) measures interference patterns, which reveal the symmetry and character of electronic excited states in the same way as elastic scattering does for the ground state. A prototypical example is provided by the quasi-molecular electronic structure of insulating Ba3CeIr2O9 with structural Ir dimers and strong spin-orbit coupling. The double "slits" in this resonant experiment are the highly localized core levels of the two Ir atoms within a dimer. The clear double-slit-type sinusoidal interference patterns that we observe allow us to characterize the electronic excitations, demonstrating the power of RIXS interferometry to unravel the electronic structure of solids containing, e.g., dimers, trimers, ladders, or other superstructures.

Study of the electronic and magnetic properties as a function of isoelectronic substitution in SmFe(1-x)RuxAsO0.85F0.15.

We have studied the electronic and magnetic properties of SmFe(1-x)RuxAsO0.85F0.15 (x = 0, 0.05, 0.25, 0.33, 0.5) by high-resolution x-ray absorption and x-ray emission spectroscopy. The local Fe magnetic moment (µ) tends to decrease for a small Ru substitution, but it shows a clear increase with further substitution. It appears that impurity scattering prevails in reducing the µ with small Ru substitution due to an extended Ru d-band. A nanoscale phase separation, that decouples the FeAs layers from the spacer layers, drives the increase of µ at higher Ru substitution. The results provide important information on nanoscale phase separation due to isoelectronic substitution in the active layers of iron-based 1111-superconductors and its effect on the local magnetic properties.

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%.

Locking of iridium magnetic moments to the correlated rotation of oxygen octahedra in Sr2IrO4 revealed by x-ray resonant scattering.

Sr2IrO4 is a prototype of the class of Mott insulators in the strong spin-orbit interaction (SOI) limit described by a Jeff = 1/2 ground state. In Sr2IrO4, the strong SOI is predicted to manifest itself in the locking of the canting of the magnetic moments to the correlated rotation by 11.8(1)° of the oxygen octahedra that characterizes its distorted layered perovskite structure. Using x-ray resonant scattering at the Ir L3 edge we have measured accurately the intensities of Bragg peaks arising from different components of the magnetic structure. From a careful comparison of integrated intensities of peaks due to basal-plane antiferromagnetism, with those due to b-axis ferromagnetism, we deduce a canting of the magnetic moments of 12.2(8)°. We thus confirm that in Sr2IrO4 the magnetic moments rigidly follow the rotation of the oxygen octahedra, indicating that, even in the presence of significant non-cubic structural distortions, it is a close realization of the Jeff = 1/2 state.

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.

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.