Evolution of the Magnetic Excitations in Electron-Doped La_{2-x}Ce_{x}CuO_{4}.

We investigated the high energy spin excitations in electron-doped La_{2-x}Ce_{x}CuO_{4}, a cuprate superconductor, by resonant inelastic x-ray scattering (RIXS) measurements. Efforts were paid to disentangle the paramagnon signal from non-spin-flip spectral weight mixing in the RIXS spectrum at Q_{∥}=(0.6π,0) and (0.9π,0) along the (1 0) direction. Our results show that, for doping level x from 0.07 to 0.185, the variation of the paramagnon excitation energy is marginal. We discuss the implication of our results in connection with the evolution of the electron correlation strength in this system.

Anisotropic hybridization probed by polarization dependent x-ray absorption spectroscopy in VI3van der Waals Mott ferromagnet.

Polarization dependent x-ray absorption spectroscopy was used to study the magnetic ground state and the orbital occupation in bulk-phase VI3van der Waals crystals below and above the ferromagnetic and structural transitions. X-ray natural linear dichroism and x-ray magnetic circular dichroism spectra acquired at the VL2,3edges are compared against multiplet cluster calculations within the frame of the ligand field theory to quantify the intra-atomic electronic interactions at play and evaluate the effects of symmetry reduction occurring in a trigonally distorted VI6unit. We observed a non zero linear dichroism proving the presence of an anisotropic charge density distribution around the V3+ion due to the unbalanced hybridization between the vanadium and the ligand states. Such hybridization acts as an effective trigonal crystal field, slightly lifting the degeneracy of thet2g2ground state. However, the energy splitting associated to the distortion underestimates the experimental band gap, suggesting that the insulating ground state is stabilized by Mott correlation effects rather than via a Jahn-Teller mechanism. Our results clarify the role of the distortion in VI3and establish a benchmark for the study of the spectroscopic properties of other van der Waals halides, including emerging 2D materials with mono and few-layers thickness, whose fundamental properties might be altered by reduced dimensions and interface proximity.

Fate of charge order in overdoped La-based cuprates.

In high-temperature cuprate superconductors, stripe order refers broadly to a coupled spin and charge modulation with a commensuration of eight and four lattice units, respectively. How this stripe order evolves across optimal doping remains a controversial question. Here we present a systematic resonant inelastic x-ray scattering study of weak charge correlations in La2-xSrxCuO4 and La1.8-xEu0.2SrxCuO4. Ultra high energy resolution experiments demonstrate the importance of the separation of inelastic and elastic scattering processes. Long-range temperature-dependent stripe order is only found below optimal doping. At higher doping, short-range temperature-independent correlations are present up to the highest doping measured. This transformation is distinct from and preempts the pseudogap critical doping. We argue that the doping and temperature-independent short-range correlations originate from unresolved electron-phonon coupling that broadly peaks at the stripe ordering vector. In La2-xSrxCuO4, long-range static stripe order vanishes around optimal doping and we discuss both quantum critical and crossover scenarios.

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.

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.

Similar temperature scale for valence changes in Kondo lattices with different Kondo temperatures.

The Kondo model predicts that both the valence at low temperatures and its temperature dependence scale with the characteristic energy TK of the Kondo interaction. Here, we study the evolution of the 4f occupancy with temperature in a series of Yb Kondo lattices using resonant X-ray emission spectroscopy. In agreement with simple theoretical models, we observe a scaling between the valence at low temperature and TK obtained from thermodynamic measurements. In contrast, the temperature scale Tv at which the valence increases with temperature is almost the same in all investigated materials while the Kondo temperatures differ by almost four orders of magnitude. This observation is in remarkable contradiction to both naive expectation and precise theoretical predictions of the Kondo model, asking for further theoretical work in order to explain our findings. Our data exclude the presence of a quantum critical valence transition in YbRh2Si2.

Magnetic bistability of a TbPc2 submonolayer on a graphene/SiC(0001) conductive electrode.

The alteration of the properties of single-molecule magnets (SMMs) due to the interaction with metallic electrodes is detrimental to their employment in spintronic devices. Conversely, herein we show that the terbium(iii) bis-phthalocyaninato complex, TbPc2, maintains its SMM behavior up to 9 K on a graphene/SiC(0001) substrate, making this alternative conductive layer highly promising for molecular spintronic applications.

Probing magnetic coupling between LnPc2 (Ln = Tb, Er) molecules and the graphene/Ni (111) substrate with and without Au-intercalation: role of the dipolar field.

Lanthanides (Ln) bis-phthalocyanine (Pc), the so-called LnPc2double decker, are a promising class of molecules with a well-defined magnetic anisotropy. In this work, we investigate the magnetic properties of LnPc2 molecules UHV-deposited on a graphene/Ni(111) substrate and how they modify when an Au layer is intercalated between Ni and graphene. X-ray absorption spectroscopy (XAS), and linear and magnetic circular dichroism (XLD and XMCD) were used to characterize the systems and probe the magnetic coupling between LnPc2 molecules and the Ni substrate through graphene, both gold-intercalated and not. Two types of LnPc2 molecules (Ln = Tb, Er) with a different magnetic anisotropy (easy-axis for Tb, easy-plane for Er) were considered. XMCD shows an antiferromagnetic coupling between Ln and Ni(111) even in the presence of the graphene interlayer. Au intercalation causes the vanishing of the interaction between Tb and Ni(111). In contrast, in the case of ErPc2, we found that the gold intercalation does not perturb the magnetic coupling. These results, combined with the magnetic anisotropy of the systems, suggest the possible importance of the magnetic dipolar field contribution for determining the magnetic behaviour.

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.

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.

Spin-communication channels between Ln(III) bis-phthalocyanines molecular nanomagnets and a magnetic substrate.

Learning the art of exploiting the interplay between different units at the atomic scale is a fundamental step in the realization of functional nano-architectures and interfaces. In this context, understanding and controlling the magnetic coupling between molecular centers and their environment is still a challenging task. Here we present a combined experimental-theoretical work on the prototypical case of the bis(phthalocyaninato)-lanthanide(III) (LnPc2) molecular nanomagnets magnetically coupled to a Ni substrate. By means of X-ray magnetic circular dichroism we show how the coupling strength can be tuned by changing the Ln ion. The microscopic parameters of the system are determined by ab-initio calculations and then used in a spin Hamiltonian approach to interpret the experimental data. By this combined approach we identify the features of the spin communication channel: the spin path is first realized by the mediation of the external (5d) electrons of the Ln ion, keeping the characteristic features of the inner 4 f orbitals unaffected, then through the organic ligand, acting as a bridge to the external world.

The high-field magnet endstation for X-ray magnetic dichroism experiments at ESRF soft X-ray beamline ID32.

A new high-field magnet endstation for X-ray magnetic dichroism experiments has been installed and commissioned at the ESRF soft X-ray beamline ID32. The magnet consists of two split-pairs of superconducting coils which can generate up to 9 T along the beam and up to 4 T orthogonal to the beam. It is connected to a cluster of ultra-high-vacuum chambers that offer a comprehensive set of surface preparation and characterization techniques. The endstation and the beam properties have been designed to provide optimum experimental conditions for X-ray magnetic linear and circular dichroism experiments in the soft X-ray range between 400 and 1600 eV photon energy. User operation started in November 2014.

Stability of the Zhang-Rice Singlet with Doping in Lanthanum Strontium Copper Oxide Across the Superconducting Dome and Above.

The spin character of the states at the top of the valence band in doped La(2-x)Sr(x)CuO(4) (x=0.03, 0.07, 0.15, 0.22, and 0.30) has been investigated using spin-polarized resonant photoemission. A clear Zhang-Rice singlet (ZRS) is observed at all doping levels. Its stability and polarization are preserved as a function of doping, suggesting that the concept of the ZRS can be used across a wide doping range and up to the metallic nonsuperconducting overdoped regime. The results are significant for theoretical models that use the ZRS approximation and for the understanding of the peculiar interplay between the ZRS and the remaining localized spins.

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.

Ubiquitous long-range antiferromagnetic coupling across the interface between superconducting and ferromagnetic oxides.

The so-called proximity effect is the manifestation, across an interface, of the systematic competition between magnetic order and superconductivity. This phenomenon has been well documented and understood for conventional superconductors coupled with metallic ferromagnets; however it is still less known for oxide materials, where much higher critical temperatures are offered by copper oxide-based superconductors. Here we show that, even in the absence of direct Cu-O-Mn covalent bonding, the interfacial CuO2 planes of superconducting La(1.85)Sr(0.15)CuO(4) thin films develop weak ferromagnetism associated to the charge transfer of spin-polarised electrons from the La(0.66)Sr(0.33)MnO(3) ferromagnet. Theoretical modelling confirms that this effect is general to all cuprate/manganite heterostructures and the presence of direct bonding only affects the strength of the coupling. The Dzyaloshinskii-Moriya interaction, also at the origin of the weak ferromagnetism of bulk cuprates, propagates the magnetisation from the interface CuO2 planes into the superconductor, eventually depressing its critical temperature.

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%.

Origin of interface magnetism in BiMnO3/SrTiO3 and LaAlO3/SrTiO3 heterostructures.

Possible ferromagnetism induced in otherwise nonmagnetic materials has been motivating intense research in complex oxide heterostructures. Here we show that a confined magnetism is realized at the interface between SrTiO3 and two insulating polar oxides, BiMnO3 and LaAlO3. By using polarization dependent x-ray absorption spectroscopy, we find that in both cases the magnetism can be stabilized by a negative exchange interaction between the electrons transferred to the interface and local magnetic moments. These local magnetic moments are associated with magnetic Ti3+ ions at the interface itself for LaAlO3/SrTiO3 and to Mn3+ ions in the overlayer for BiMnO3/SrTiO3. In LaAlO3/SrTiO3 the induced magnetism is quenched by annealing in oxygen, suggesting a decisive role of oxygen vacancies in this phenomenon.