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Complex oxides are well known to develop oxygen ordering patterns with well defined periodicities, but their interplay with electronic correlations remains largely unexplored. Here, we report resonant and non-resonant x-ray diffraction data indicating a four-unit-cell periodic superstructure related to oxygen vacancy ordering in La$_{2-x}$Ca$_{x}$CuO$_{4}$ films with doping levels from the underdoped ($x = 0.15$) to the extremely overdoped ($x = 0.50$) regime. Whereas the lattice superstructure is temperature independent up to 300 K, a strongly temperature dependent electronic charge density wave (CDW) is observed in the underdoped and slightly overdoped regimes ($x\leq0.20$). The periodicity, in-plane and out-of-plane correlation lengths of the CDW are locked in by the lattice superstructure. Our results highlight the necessity to consider lattice and electronic energetics on equal footing in the high-temperature oxygen-disordered phase to explain oxygen ordering phenomena in complex oxides., Comment: 4 figures, supplement included

Van der Waals materials provide a versatile toolbox for the emergence of new quantum phenomena and the fabrication of functional heterostructures. Among them, the trihalide VI3 stands out for its unique magnetic and structural landscape. Here we investigate the spin and orbital magnetic degrees of freedom in the layered ferromagnet VI3 by means of temperature-dependent x-ray absorption spectroscopy and x-ray magnetic circular and linear dichroism. We detect localized electronic states and reduced magnetic dimensionality, due to electronic correlations. We furthermore provide experimental evidence of (a) an unquenched orbital magnetic moment (up to 0.66(7)) in the ferromagnetic state, and (b) an instability of the orbital moment in proximity of the spin reorientation transition. Our results support a coherent picture where electronic correlations give rise to a strong magnetic anisotropy and a large orbital moment, and establish VI3 as a prime candidate for the study of orbital quantum effects.

The essential building blocks of cuprate superconductors are two-dimensional CuO$_2$ sheets interspersed with charge reservoir layers. In bilayer cuprates, two closely spaced CuO$_2$ sheets are separated by a larger distance from the subsequent pair in the next unit cell. In contrast to single-layer cuprates, prior theoretical work on bilayer systems has predicted two distinct acoustic plasmon bands for a given out-of-plane momentum transfer. Here we report random phase approximation (RPA) calculations for bilayer systems which corroborate the existence of two distinct plasmons bands. We find that the intensity of the lower-energy band is negligibly small, whereas the higher-energy band carries significant spectral weight. We also present resonant inelastic x-ray scattering (RIXS) experiments at the O $K$-edge on the bilayer cuprate Y$_{0.85}$Ca$_{0.15}$Ba$_2$Cu$_3$O$_7$ (Ca-YBCO), which show only one dispersive plasmon branch, in agreement with the RPA calculations. In addition, the RPA results indicate that the dispersion of the higher-energy plasmon band in Ca-YBCO is not strictly acoustic, but exhibits a substantial energy gap of approximately 250 meV at the two-dimensional Brillouin zone center., Comment: 9 pages, 7 figures

We investigated the high energy spin excitations in electron-doped $\mathrm{La}_{2-x} \mathrm{Ce}_x \mathrm{CuO}_{4}$, 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 $\bf{Q_{\|}}$ = $(0.6\pi, 0)$ and $(0.9\pi, 0)$ 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., Comment: in press on Phys. Rev. Lett

Magnetic frustration is a route that can lead to the emergence of novel ground states, including spin liquids and spin ices. Such frustration can be introduced through either the geometry of lattice structures or by incompatible exchange interactions. Identifying suitable strategies to control the degree of magnetic frustration in real systems is an active field of research. In this study, we devise a design principle for the tuning of frustrated magnetism on the square lattice through the manipulation of nearest (NN) and next-nearest neighbor (NNN) antiferromagnetic (AF) exchange interactions. By studying the magnon excitations in epitaxially-strained La$_2$NiO$_4$ films using resonant inelastic x-ray scattering (RIXS) we show that, in contrast to the cuprates, the dispersion peaks at the AF zone boundary. This indicates the presence of an AF-NNN spin interaction. Using first principles simulations and an effective spin-model, we demonstrate the AF-NNN coupling to be a consequence of the two-orbital nature of La$_2$NiO$_4$. Our results demonstrate that compressive strain can enhance this coupling, providing a design principle for the tunability of frustrated magnetism on a square lattice.

Polarization dependent x-ray absorption spectroscopy was used to study the magnetic ground state and the orbital occupation in bulk-phase VI$_3$ van 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 V $L_{2,3}$ edges 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 VI$_6$ unit. We observed a non zero linear dichroism proving the presence of an anisotropic charge density distribution around the V$^{3+}$ 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 the $t_{2g}^2$ ground 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 VI$_3$ and 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.

The universality of the strange metal phase in many quantum materials is often attributed to the presence of a quantum critical point (QCP), a zero-temperature phase transition ruled by quantum fluctuations. In cuprates, where superconductivity hinders direct QCP observation, indirect evidence comes from the identification of fluctuations compatible with the strange metal phase. Here we show that the recently discovered charge density fluctuations (CDF) possess the right properties to be associated to a quantum phase transition. Using resonant x-ray scattering, we studied the CDF in two families of cuprate superconductors across a wide doping range (up to $p$=0.22). At $p^*\approx$0.19, the putative QCP, the CDF intensity peaks, and the characteristic energy $\Delta$ is minimum, marking a wedge-shaped region in the phase diagram indicative of a quantum critical behavior, albeit with anomalies. These findings strengthen the role of charge order in explaining strange metal phenomenology and provide insights into high-temperature superconductivity., Comment: 36 pages, 4 figures, 9 supplementary figures

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 (RIXS) study of weak charge correlations in La2-xSrxCuO4 (LSCO) and La1.8-xEu0.2SrxCuO4 (LESCO). Ultra high energy resolution experiments demonstrate the importance of the separation of inelastic and elastic scattering processes. Upon increasing doping x, the long-range temperature dependent stripe order is found to be replaced by short-range temperature independent correlations at a critical point xc = 0.15 distinct from 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 LSCO, long-range static stripe order vanishes in a quantum critical point around optimal doping.

Bulk charge density waves are now reported in nearly all high-temperature superconducting cuprates, with the noticeable exception of one particular family: the copper oxychlorides. Here, we used resonant inelastic X-ray scattering to reveal a bulk charge density waves in these materials. Combining resonant inelastic X-ray scattering with non-resonant inelastic X-ray scattering, we investigate the interplay between the lattice excitations and the charge density wave, and evidence the phonon anomalies of the Cu-O bond-stretching mode at the charge density wave wave-vector. We propose that such electron-phonon anomalies occur in the presence of dispersive charge excitations emanating from the charge density wave and interacting with the Cu-O bond-stretching phonon. Our results pave the way for future studies, combining both bulk and surface probes, to investigate the static and dynamical properties of the charge density wave in the copper oxychloride family.

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 (RIXS) 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. In addition, we detect an elastic resonant scattering peak in the uncapped $x=0$ compound at wave vector (1/3,0), 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 uncapped samples also present a higher degree of Ni$3d$-Nd$5d$ hybridization and a smaller anisotropy of the Ni$3d$ occupation with respect to the capped samples. The role of the capping on the possible hydrogen incorporation or on other mechanisms responsible for the electronic reconstruction far from the interface remains to be understood.

We report on a novel material, namely two-dimensional (2D) V$_{1-x}$Pt$_x$Se$_2$ alloy, exhibiting simultaneously ferromagnetic order and Rashba spin-orbit coupling. While ferromagnetism is absent in 1T-VSe$_2$ due to the competition with the charge density wave phase, we demonstrate theoretically and experimentally that the substitution of vanadium by platinum in VSe$_2$ (10-50 %) to form an homogeneous 2D alloy restores ferromagnetic order with Curie temperatures of 6 K for 5 monolayers and 25 K for one monolayer of V$_{0.65}$Pt$_{0.35}$Se$_2$. Moreover, the presence of platinum atoms gives rise to Rashba spin-orbit coupling in (V,Pt)Se$_2$ providing an original platform to study the interplay between ferromagnetism and spin-orbit coupling in the 2D limit., Comment: 5 pages, 5 figures

The normal state of optimally doped cuprates is dominated by the "strange metal" phase that shows a linear temperature ($T$) dependence of the resistivity persisting down to the lowest $T$. For underdoped cuprates this behavior is lost below the pseudogap temperature $T^*$, where Charge Density Waves (CDW) together with other intertwined local orders characterize the ground state. Here we show that the $T$-linear resistivity of highly strained, ultrathin and underdoped YBa$_2$Cu$_3$O$_{7-\delta}$ films is restored when the CDW amplitude, detected by Resonant Inelastic X-ray scattering, is suppressed. This observation points towards an intimate connection between the onset of CDW and the departure from $T$-linear resistivity in underdoped cuprates. Our results illustrate the potential of using strain control to manipulate the ground state of quantum materials.

We report a comprehensive Cu L$_3$-edge resonant x-ray scattering 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. The pressure response of the 2D charge correlations is symmetric: 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 resonant x-ray scattering 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., Comment: Revised version - Accepted for publication in Phys. Rev. Lett

The charge-density-wave (CDW) instability in the underdoped, pseudogap part of the cuprate phase diagram has been a major recent research focus, yet measurements of dynamic, energy-resolved CDW correlations are still in their infancy. We report a high-resolution resonant inelastic X-ray scattering (RIXS) study of the underdoped cuprate superconductor HgBa$_{2}$CuO$_{4+\delta}$ ($T_c = 70$ K). At $T=250$ K, above the CDW order temperature $T_\mathrm{CDW} \approx 200$ K, we observe significant dynamic CDW correlations at about 40 meV. This energy scale is comparable to both the superconducting gap and the previously reported low-energy pseudogap. At $T = T_c$, a strong elastic CDW peak appears, but the dynamic correlations around 40 meV remain virtually unchanged. In addition, we observe a new feature: dynamic correlations at significantly higher energy, with a characteristic scale of about 160 meV. A similar scale was previously identified in other experiments as a high-energy pseudogap. The existence of three distinct features in the charge response is highly unusual for a CDW system, and suggests that charge order in the cuprates is closely related to the pseudogap phenomenon and more complex than previously thought. We further observe the paramagnon dispersion along [1,0], across the two-dimensional CDW wavevector $\boldsymbol{q}_\mathrm{CDW}$, which is consistent with magnetic excitations measured by inelastic neutron scattering. Unlike for some other cuprates, our results point to the absence of a discernible coupling between CDW and magnetic excitations.

Although charge density waves (CDWs) are omnipresent in cuprate high-temperature superconductors, they occur at significantly different wavevectors, confounding efforts to understand their formation mechanism. Here, we use resonant inelastic x-ray scattering to investigate the doping- and temperature-dependent CDW evolution in La2-xBaxCuO4 (x=0.115-0.155). We discovered that the CDW develops in two stages with decreasing temperature. A precursor CDW with quasi-commensurate wavevector emerges first at high-temperature. This doping-independent precursor CDW correlation originates from the CDW phase mode coupled with a phonon and "seeds" the low-temperature CDW with strongly doping dependent wavevector. Our observation reveals the precursor CDW and its phase mode as the building blocks of the highly intertwined electronic ground state in the cuprates., Comment: In press at Physical Review X; 11 pages, 6 figures

We have studied the electronic structure of BaCoO$_3$ using soft x-ray absorption spectroscopy at the Co-$L_{2,3}$ and O-$K$ edges, magnetic circular dichroism at the Co-$L_{2,3}$ edges, as well as valence band hard x-ray photoelectron spectroscopy. The quantitative analysis of the spectra established that the Co ions are in the formal low-spin tetravalent 3$d^5$ state and that the system is a negative charge transfer Mott insulator. The spin-orbit coupling plays also an important role for the magnetism of the system. At the same time, a trigonal crystal field is present with sufficient strength to bring the 3$d^5$ ion away from the $J_{eff} = 1/2$ state. The sign of this crystal field is such that the $a_{1g}$ orbital is doubly occupied, explaining the absence of a Peierl's transition in this system which consists of chains of face-sharing CoO$_6$ octahedra. Moreover, with one hole residing in the $e_g^{\pi}$, the presence of an orbital moment and strong magneto-crystalline anisotropy can be understood. Yet, we also infer that crystal fields with lower symmetry must be present to reproduce the measured orbital moment quantitatively, thereby suggesting the possibility for orbital ordering to occur in BaCoO$_3$.

We used high-resolution resonant inelastic x-ray scattering (RIXS) at the Ni $L_3$ edge to simultaneously investigate high-energy interband transitions characteristic of Ni-O bond ordering and low-energy collective excitations of the Ni spins in the rare-earth nickelates $R$NiO$_3$ ($R$ = Nd, Pr, La) with pseudocubic perovskite structure. With the support of calculations based on a double-cluster model we quantify bond order (BO) amplitudes for different thin films and heterostructures and discriminate short-range BO fluctuations from long-range static order. Moreover we investigate magnetic order and exchange interactions in spatially confined $R$NiO$_3$ slabs by probing dispersive magnon excitations. While our study of superlattices (SLs) grown in the (001) direction of the perovskite structure reveals a robust non-collinear spin spiral magnetic order with dispersive magnon excitations that are essentially unperturbed by BO modulations and spatial confinement, we find magnons with flat dispersions and strongly reduced energies in SLs grown in the $(111)_{\text{pc}}$ direction that exhibit collinear magnetic order. These results give insight into the interplay of different collective ordering phenomena in a prototypical 3$d$ transition metal oxide and establish RIXS as a powerful tool to quantitatively study several order parameters and the corresponding collective excitations within one experiment., Comment: 13 pages, 8 figures, accepted in Physical Review B

High resolution resonant inelastic x-ray scattering (RIXS) has proven particularly effective in the determination of crystal field and spin excitations in cuprates. Its strength lies in the large Cu $L_{3}$ resonance and in the fact that the scattering cross section follows quite closely the single-ion model predictions, both in the insulating parent compounds and in the superconducting doped materials. However, the spectra become increasingly broader with (hole) doping, hence resolving and assigning spectral features has proven challenging even with the highest energy resolution experimentally achievable. Here we have overcome this limitation by measuring the complete polarization dependence of the RIXS spectra as function of momentum transfer and doping in thin films of NdBa$_{2}$Cu$_{3}$O$_{7-\delta}$. Besides confirming the previous assignment of $dd$ and spin excitations (magnon, bimagnon) in the antiferromagnetic insulating parent compound, we unequivocally single out the actual spin-flip contribution at all dopings. We also demonstrate that the softening of $dd$ excitations is mainly attributed to the shift of the $xy$ peak to lower energy loss. These results provide a definitive assessment of the RIXS spectra of cuprates and demonstrate that RIXS measurements with full polarization control are practically feasible and highly informative., Comment: 14 pages, 10 figures

High temperature cuprate superconductors consist of stacked CuO2 planes, with primarily two dimensional electronic band structures and magnetic excitations, while superconducting coherence is three dimensional. This dichotomy highlights the importance of out-of-plane charge dynamics, believed to be incoherent in the normal state, yet lacking a comprehensive characterization in energy-momentum space. Here, we use resonant inelastic x-ray scattering (RIXS) with polarization analysis to uncover the pure charge character of a recently discovered collective mode in electron-doped cuprates. This mode disperses along both the in- and, importantly, out-of-plane directions, revealing its three dimensional nature. The periodicity of the out-of-plane dispersion corresponds to the CuO2 plane distance rather than the crystallographic c-axis lattice constant, suggesting that the interplane Coulomb interaction drives the coherent out-of-plane charge dynamics. The observed properties are hallmarks of the long-sought acoustic plasmon, predicted for layered systems and argued to play a substantial role in mediating high temperature superconductivity., Comment: This is the version of first submission. The revised manuscript according to peer reviews is now accepted by Nature and will be published online on 31st Oct., 2018

Charge density waves are a common occurrence in all families of high critical temperature superconducting cuprates. Although consistently observed 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 (Y,Nd)Ba$_2$Cu$_3$O$_{7-{\delta}}$ for three doping levels. We discovered short-range dynamical charge density fluctuations besides the previously known quasi-critical charge density waves. They persist up to well above the pseudogap temperature T*, are characterized by energies of few meV and pervade a large area of the phase diagram, so that they can play a key role in shaping the peculiar normal-state properties of cuprates., Comment: 34 pages, 4 figures, 11 supplementary figures

We report an Fe $L$-edge resonant inelastic x-ray scattering (RIXS) study of the unusual superconductor $\beta$-FeSe. The high energy resolution of this RIXS experiment ($\approx\,$55$\,$meV FWHM) made it possible to resolve low-energy excitations of the Fe $3d$ manifold. These include a broad peak which shows dispersive trends between 100-200$\,$meV along the $(\pi,0)$ and $(\pi,\pi)$ directions of the one-Fe square reciprocal lattice, and which can be attributed to paramagnon excitations. The multi-band valence state of FeSe is among the most metallic in which such excitations have been discerned by soft x-ray RIXS.

Using Cu-$L_3$ edge resonant inelastic x-ray scattering (RIXS) we measured the dispersion and damping of spin excitations (magnons and paramagnons) in the high-$T_\mathrm{c}$ superconductor (Bi,Pb)$_{2}$(Sr,La)$_{2}$CuO$_{6+\delta}$ (Bi2201), for a large doping range across the phase diagram ($0.03\lesssim p\lesssim0.21$). Selected measurements with full polarization analysis unambiguously demonstrate the spin-flip character of these excitations, even in the overdoped sample. We find that the undamped frequencies increase slightly with doping for all accessible momenta, while the damping grows rapidly, faster in the (0,0)$\rightarrow$(0.5,0.5) nodal direction than in the (0,0)$\rightarrow$(0.5,0) antinodal direction. We compare the experimental results to numerically exact determinant quantum Monte Carlo (DQMC) calculations that provide the spin dynamical structure factor $S(\textbf{Q},\omega)$ of the three-band Hubbard model. The theory reproduces well the momentum and doping dependence of the dispersions and spectral weights of magnetic excitations. These results provide compelling evidence that paramagnons, although increasingly damped, persist across the superconducting dome of the cuprate phase diagram; this implies that long range antiferromagnetic correlations are quickly washed away, while short range magnetic interactions are little affected by doping., Comment: 11 pages, 9 figures

We have used high-resolution resonant inelastic x-ray scattering (RIXS) to study a thin film of NdNiO$_3$, a compound whose unusual spin- and bond-ordered electronic ground state has been of long-standing interest. Below the magnetic ordering temperature, we observe well-defined collective magnon excitations along different high-symmetry directions in momentum space. The magnetic spectra depend strongly on the incident photon energy, which we attribute to RIXS coupling to different local electronic configurations of the expanded and compressed NiO$_6$ octahedra in the bond-ordered state. Both the noncollinear magnetic ground state and the observed site-dependent magnon excitations are well described by a model that assumes strong competition between the antiferromagnetic superexchange and ferromagnetic double-exchange interactions. Our study provides direct insight into the magnetic dynamics and exchange interactions of the rare-earth nickelates, and demonstrates that RIXS can serve as a site-selective probe of magnetism in these and other materials., Comment: Phys. Rev. X, in press

We used x-ray absorption spectroscopy to study the orbital symmetry and the energy band splitting of (111) LaAlO${_3}$/SrTiO${_3}$ and LaAlO${_3}$/EuTiO${_3}$/SrTiO${_3}$ heterostructures, hosting a quasi two-dimensional electron system (q2DES), and of a Ti-terminated (111) SrTiO${_3}$ single crystal, also known to form a q2DES at its surface. We demonstrate that the bulk tetragonal Ti-3d D${_4}$${_h}$ crystal field is turned into trigonal D${_3}$${_d}$ crystal field in all cases. The symmetry adapted a${_1}$${_g}$ and e${^\pi_g}$ orbitals are non-degenerate in energy and their splitting, \Delta, is positive at the bare STO surface but negative in the heterostructures, where the a${_1}$${_g}$ orbital is lowest in energy. These results demonstrate that the interfacial symmetry breaking induced by epitaxial engineering of oxide interfaces has a dramatic effect on their electronic properties, and it can be used to manipulate the ground state of the q2DES., Comment: 6 pages article, plus 5 pages supplementary information

Charge order has now been observed in several cuprate high-temperature superconductors. We report a resonant inelastic x-ray scattering experiment on the electron-doped cuprate Nd$_{2-x}$Ce$_{x}$CuO$_4$ that demonstrates the existence of dynamic correlations at the charge order wave vector. Upon cooling we observe a softening in the electronic response, which has been predicted to occur for a d-wave charge order in electron-doped cuprates. At low temperatures, the energy range of these excitations coincides with that of the dispersive magnetic modes known as paramagnons. Furthermore, measurements where the polarization of the scattered photon is resolved indicate that the dynamic response at the charge order wave vector primarily involves spin-flip excitations. Overall, our findings indicate a coupling between dynamic magnetic and charge-order correlations in the cuprates., Comment: Supplementary information available upon request

The magnetic properties of rare earth compounds are usually well captured by assuming a fully localized f shell and only considering the Hund's rule ground state multiplet split by a crystal electrical field (CEF). Currently, the standard technique for probing CEF excitations in lanthanides is inelastic neutron scattering. Here we show that with the recent leap in energy resolution, resonant inelastic soft X-ray scattering has become a serious alternative for looking at CEF excitations with some distinct advantages compared to INS. As an example we study the CEF scheme in CeRh2Si2, a system that has been intensely studied for more than two decades now but for which no consensus has been reached yet as to its CEF scheme. We used two new features that have only become available very recently in RIXS, high energy resolution of about 30 meV as well as polarization analysis in the scattered beam, to find a unique CEF description for CeRh2Si2. The result agrees well with previous INS and magnetic susceptibility measurements. Due to its strong resonant character, RIXS is applicable to very small samples, presents very high cross sections for all lanthanides, and further benefits from the very weak coupling to phonon excitation. The rapid progress in energy resolution of RIXS spectrometers is making this technique increasingly attractive for the investigation of the CEF scheme in lanthanides.

The quantum anomalous Hall effect (QAHE) has recently been reported to emerge in magnetically-doped topological insulators. Although its general phenomenology is well established, the microscopic origin is far from being properly understood and controlled. Here we report on a detailed and systematic investigation of transition-metal (TM)-doped Sb$_2$Te$_3$. By combining density functional theory (DFT) calculations with complementary experimental techniques, i.e., scanning tunneling microscopy (STM), resonant photoemission (resPES), and x-ray magnetic circular dichroism (XMCD), we provide a complete spectroscopic characterization of both electronic and magnetic properties. Our results reveal that the TM dopants not only affect the magnetic state of the host material, but also significantly alter the electronic structure by generating impurity-derived energy bands. Our findings demonstrate the existence of a delicate interplay between electronic and magnetic properties in TM-doped TIs. In particular, we find that the fate of the topological surface states critically depends on the specific character of the TM impurity: while V- and Fe-doped Sb$_2$Te$_3$ display resonant impurity states in the vicinity of the Dirac point, Cr and Mn impurities leave the energy gap unaffected. The single-ion magnetic anisotropy energy and easy axis, which control the magnetic gap opening and its stability, are also found to be strongly TM impurity-dependent and can vary from in-plane to out-of-plane depending on the impurity and its distance from the surface. Overall, our results provide general guidelines for the realization of a robust QAHE in TM-doped Sb$_2$Te$_3$ in the ferromagnetic state., Comment: 40 pages, 13 figures

Spin excitations in the overdoped high temperature superconductors Tl$_2$Ba$_2$CuO$_{6+\delta}$ and (Bi,Pb)$_2$(Sr,La)$_{2}$CuO$_{6+\delta}$ 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 fluorescence-like 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., Comment: 6 pages, 3 figures, accepted in Physical Review Letters

Charge modulations are considered as a leading competitor of high-temperature superconductivity in the underdoped cuprates, and their relationship to Fermi surface reconstructions and to the pseudogap state is an important subject of current research. Overdoped cuprates, on the other hand, are widely regarded as conventional Fermi liquids without collective electronic order. For the overdoped (Bi,Pb)2.12Sr1.88CuO6+{\delta} (Bi2201) high-temperature superconductor, here we report resonant x-ray scattering measurements revealing incommensurate charge order reflections, with correlation lengths of 40-60 lattice units, that persist up to at least 250K. Charge order is markedly more robust in the overdoped than underdoped regime but the incommensurate wave vectors follow a common trend; moreover it coexists with a single, unreconstructed Fermi surface, without pseudogap or nesting features, as determined from angle-resolved photoemission spectroscopy. This re-entrant charge order is reproduced by model calculations that consider a strong van Hove singularity within a Fermi liquid framework., Comment: 11 pages, 5 figures

Ferrimagnetic Mn$_2$Fe$_x$Ga $(0.26 \leq x \leq 1.12)$ thin films have been characterised by X-ray diffraction, SQUID magnetometry, X-ray absorption spectroscopy, X-ray magnetic circular dichroism and M\"{o}ssbauer spectroscopy with the aim of determining the structure and site-specific magnetism of this tetragonal, D0$_{22}$-structure Heusler compound. High-quality epitaxial films with low RMS surface roughness ($\sim 0.6$ nm) are grown by magnetron co-sputtering. The tetragonal distortion induces strong perpendicular magnetic anisotropy along the $c$-axis with a typical coercive field $\mu_0 H\sim 0.8$ T and an anisotropy field ranging from $6$ to $8$ T. Upon increasing the Fe content $x$, substantial uniaxial anisotropy, $K_\mathrm{u} \geq 1.0$ MJ/m$^3$ can be maintained over the full $x$ range, while the magnetisation of the compound is reduced from $400$ to $280$ kA/m. The total magnetisation is almost entirely given by the sum of the spin moments originating from the ferrimagnetic Mn and Fe sublattices, with the latter being coupled ferromagnetically to one of the former. The orbital magnetic moments are practically quenched, and have negligible contributions to the magnetisation. The films with $x=0.73$ exhibit a high anomalous Hall angle of $2.5$ % and a high Fermi-level spin polarisation, above $51$ %, as measured by point contact Andreev reflection. The Fe-substituted Mn$_2$Ga films are highly tunable with a unique combination of high anisotropy, low magnetisation, appreciable spin polarisation and low surface roughness, making them very strong candidates for thermally-stable spin-transfer-torque switching nanomagnets with lateral dimensions down to $10$ nm., Comment: 11 pages, 11 figures

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 (RIXS) to follow the evolution of charge correlations in the canonical stripe ordered cuprate La$_{1.875}$Ba$_{0.125}$CuO$_{4}$ (LBCO~$1/8$) 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., Comment: Accepted in Proceeding of the National Academy of Sciences; 8 pages, 4 figures

The Kondo model predicts that both the valence at low temperatures and its temperature dependence scale with the characteristic energy T_K 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 T_K obtained from thermodynamic measurements. In contrast, the temperature scale T_v 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.

Charge order in underdoped and optimally doped high-$T_\mathrm{c}$ superconductors Bi$_{2}$Sr$_{2-x}$La$_x$CuO$_{6+\delta}$ (Bi2201) is investigated by Cu $L_3$ edge resonant inelastic x-ray scattering (RIXS). We have directly observed charge density modulation in the optimally doped Bi2201 at momentum transfer $Q_{\|} \simeq 0.23$ rlu, with smaller intensity and correlation length with respect to the underdoped sample. This demonstrates that short-range charge order in Bi2201 persists up to optimal doping, as in other hole-doped cuprates. We explored the nodal (diagonal) direction and found no charge order peak, confirming that charge order modulates only along the Cu-O bond directions. We measured the out-of-plane dependence of charge order, finding a flat response and no maxima at half integer \emph{L} values. This suggests there is no out-of-plane phase correlation in single layer Bi2201, at variance from YBa$_2$Cu$_3$O$_{6+x}$ and La$_{2-x}$(Ba,Sr)$_x$CuO$_4$. Combining our results with data from the literature we assess that charge order in Bi2201 exists in a large doping range across the phase diagram, i.e. $0.07 \lesssim p \lesssim 0.16$, demonstrating thereby that it is intimately entangled with the antiferromagnetic background, the pseudogap and superconductivity., Comment: 9 pages, 7 figures

In high Tc superconductors the magnetic and electronic properties are determined by the probability that valence electrons virtually jump from site to site in the CuO2 planes, a mechanism opposed by on-site Coulomb repulsion and favored by hopping integrals. The spatial extent of the latter is related to transport properties, including superconductivity, and to the dispersion relation of spin excitations (magnons). Here, for three antiferromagnetic parent compounds (single-layer Bi2Sr0.99La1.1CuO6+delta, double-layer Nd1.2Ba1.8Cu3O6 and infinite-layer CaCuO2) differing by the number of apical atoms, we compare the magnetic spectra measured by resonant inelastic x-ray scattering over a significant portion of the reciprocal space and with unprecedented accuracy. We observe that the absence of apical oxygens increases the in-plane hopping range and, in CaCuO2, it leads to a genuine 3D exchange-bond network. These results establish a corresponding relation between the exchange interactions and the crystal structure, and provide fresh insight into the materials dependence of the superconducting transition temperature., Comment: 9 pages, 4 figures, 1 Table, 42 references

Polar catastrophe at the interface of oxide materials with strongly correlated electrons has triggered a flurry of new research activities. The expectations are that the design of such advanced interfaces will become a powerful route to engineer devices with novel functionalities. Here we investigate the initial stages of growth and the electronic structure of the spintronic Fe3O4/MgO (001) interface. Using soft x-ray absorption spectroscopy we have discovered that the so-called A-sites are completely missing in the first Fe3O4 monolayer. This allows us to develop an unexpected but elegant growth principle in which during deposition the Fe atoms are constantly on the move to solve the divergent electrostatic potential problem, thereby ensuring epitaxy and stoichiometry at the same time. This growth principle provides a new perspective for the design of interfaces., Comment: 30 pages

Magnetic excitations in the optimally doped high-$T_\mathrm{c}$ superconductor Bi$_{1.5}$Pb$_{0.55}$Sr$_{1.6}$La$_{0.4}$CuO$_{6+\delta}$ (OP-Bi2201, $T_\mathrm{c}\simeq 34$ K) are investigated by Cu $L_3$ edge resonant inelastic x-ray scattering (RIXS), below and above the pseudogap opening temperature. At both temperatures the broad spectral distribution disperses along the (1,0) direction up to $\sim$350~meV at zone boundary, similarly to other hole-doped cuprates. However, above $\sim$0.22 reciprocal lattice units, we observe a concurrent intensity decrease for magnetic excitations and quasi-elastic signals with weak temperature dependence. This anomaly seems to indicate a coupling between magnetic, lattice and charge modes in this compound. We also compare the magnetic excitation spectra near the anti-nodal zone boundary in the single layer OP-Bi2201 and in the bi-layer optimally doped Bi$_{1.5}$Pb$_{0.6}$Sr$_{1.54}$CaCu$_2$O$_{8+\delta}$ (OP-Bi2212, $T_\mathrm{c}\simeq96$ K). The strong similarities in the paramagnon dispersion and in their energy at zone boundary indicate that the strength of the super-exchange interaction and the short-range magnetic correlation cannot be directly related to $T_\mathrm{c}$, not even within the same family of cuprates.

The strong spin-orbit interaction in the rare-earth elements ensures that even within a ferromagnetic state there is a substantial orbital contribution to the ferromagnetic moment, in contrast to more familiar transition metal systems, where the orbital moment is usually quenched. The orbital-dominant magnetization that is then possible within rare-earth systems facilitates the fabrication of entirely new magnetic heterostructures, and here we report a study of a particularly striking example comprising interfaces between GdN and SmN. Our investigation reveals a twisted magnetization arising from the large spin-only magnetic moment in GdN and the nearly zero, but orbital-dominant, moment of SmN. The unusual twisted phase is driven by (i) the similar ferromag- netic Gd-Gd, Sm-Sm and Gd-Sm exchange interactions, (ii) a SmN Zeeman interaction 200 times weaker than that of GdN, and (iii) the orbital-dominant SmN magnetic moment. The element specificity of X-ray magnetic circular dichroism (XMCD) is used in seperate modes probing both bulk and surface regions, revealing the depth profile of the twisting magnetization., Comment: 15 pages, 4 figures, supplementary material

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 YBa2Cu3O6+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., Comment: Supplementary materials are available upon request

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 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; 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%., Comment: 26 pages, 8 figures

Non-resonant Raman spectroscopy in the hard X-ray regime has been used to explore the electronic structure of the first two members of the Ruddlesden-Popper series Sr$_{n+1}$Ir$_n$O$_{3n+1}$ of iridates. By tuning the photon energy transfer around 530 eV we have been able to explore the oxygen K near edge structure with bulk sensitivity. The angular dependence of the spectra has been exploited to assign features in the 528-535 eV energy range to specific transitions involving the Ir 5d orbitals. This has allowed us to extract reliable values for both the t2g-eg splitting arising from the cubic component of the crystal field (10Dq), in addition to the splitting of the eg orbitals due to tetragonal distortions. The values we obtain are (3.8, 1.6) eV and (3.55, 1.9) eV for Sr$_2$IrO$_4$ and Sr$_3$Ir$_2$O$_7$, respectively., Comment: 6 pages, 4 figures, 2 tables

The electronic configurations of Fe, Co, Ni, and Cu adatoms on graphene and graphite have been studied by x-ray magnetic circular dichroism and charge transfer multiplet theory. A delicate interplay between long-range interactions and local chemical bonding is found to influence the adatom equilibrium distance and magnetic moment. The results for Fe and Co are consistent with purely physisorbed species having, however, different 3$d$-shell occupancies on graphene and graphite ($d^{n+1}$ and $d^n$, respectively). On the other hand, for the late 3$d$ metals Ni and Cu a trend towards chemisorption is found, which strongly quenches the magnetic moment on both substrates., Comment: 7 pages, 4 figures

Bulk charge density modulations, recently observed in high critical-temperature ($T_\mathrm{c}$) cuprate superconductors, coexist with the so-called pseudogap and compete with superconductivity. However, its direct observation has been limited to a narrow doping region in the underdoped regime. Using energy-resolved resonant x-ray scattering we have found evidence for such bulk charge modulations, or soft collective charge modes (soft CCMs), in optimally doped Bi$_{1.5}$Pb$_{0.6}$Sr$_{1.54}$CaCu$_{2}$O$_{8+\delta}$ (Pb-Bi2212) around the summit of the superconducting dome with momentum transfer $q_{\parallel}\sim0.28$ reciprocal lattice units (r.l.u.) along the Cu-O bond direction. The signal is stronger at $T\simeq T_\mathrm{c}$ than at lower temperatures, thereby confirming a competition between soft CCMs and superconductivity. These results demonstrate that soft CCMs are not constrained to the underdoped regime, suggesting that soft CCMs appear across a large part of the phase diagram of cuprates and are intimately entangled with high-$T_\mathrm{c}$ superconductivity., Comment: 6 pages, 3 figures, 1 table

The nature of the electronic groundstate of Ba2IrO4 has been addressed using soft X-ray absorption and inelastic scattering techniques in the vicinity of the oxygen K edge. From the polarization and angular dependence of XAS we deduce an approximately equal superposition of xy, yz and zx Ir4+ 5d orbitals. By combining the measured orbital occupancies, with the value of the spin-orbit coupling provided by RIXS, we estimate the crystal field splitting associated with the tetragonal distortion of the IrO6 octahedra to be small, \Delta=50(50) meV. We thus conclude definitively that Ba2IrO4 is a close realization of a spin-orbit Mott insulator with a jeff = 1/2 groundstate, thereby overcoming ambiguities in this assignment associated with the interpretation of X-ray resonant scattering experiments., Comment: 5 pages, 5 figures

The 4f crystal-electric field ground state wave functions of CeRh(1-x)Ir(x)In5 have been determined by linear polarization dependent soft x-ray absorption spectroscopy (XAS) at T = 8 K. We demonstrate that these ground state wave functions correlate with the phase diagram of the substitution series, which covers long-range antiferromagnetic order, unconventional superconductivity, and coexistence of these two states. We discuss how certain wave functions could affect magnetic order and anisotropic hybridization, facilitating the formation of a superconducting ground state at low temperatures.

We present a combined experimental and theoretical study on the local magnetism of the Co ions in the spin-chain compound CoV2O6, which crystallizes in two different allotropic phases, alpha- and gamma-CoV2O6. Using x-ray magnetic circular dichroism, we have found a very large and a moderate orbital contribution to the magnetism in alpha- and gamma-CoV2O6, respectively. Full-multiplet calculations indicate that the differences in the magnetic behavior of alpha- and gamma-CoV2O6 phases originate from different local distortions of the CoO6 octahedra. In particular, the strong compression of the CoO6 octahedra in alpha-CoV2O6 lead to a strong mixture of t2g and eg orbitals which, via the local atomic Coulomb and exchange interactions, results in an exceptionally large orbital moment.