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Confocal Raman microscopy, a highly specific and label-free technique for the microscale study of thick samples, often presents difficulties due to weak Raman signals. Inhomogeneous samples introduce wavefront aberrations that further reduce these signals, requiring even longer acquisition times. In this study, we introduce adaptive optics to confocal Raman microscopy for the first time to counteract such aberrations, significantly increasing the Raman signal and image quality. The method is designed to integrate seamlessly with existing commercial microscopes without hardware modifications. It uses a wavefront sensorless approach to derive aberrations using an optofluidic, transmissive spatial light modulator that can be attached to the microscope nosepiece. Our experimental results demonstrate the compensation of aberrations caused by artificial scatterers and mouse brain tissue, improving spatial resolution and achieving up to 3.5-fold signal enhancements. Our results provide a basis for the molecular label-free study of biological systems at greater imaging depths.

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.

Effective models focused on pertinent low-energy degrees of freedom have substantially contributed to our qualitative understanding of quantum materials. An iconic example, the Kondo model, was key to demonstrating that the rich phase diagrams of correlated metals originate from the interplay of localized and itinerant electrons. Modern electronic structure calculations suggest that to achieve quantitative material-specific models, accurate consideration of the crystal field and spin-orbit interactions is imperative. This poses the question of how local high-energy degrees of freedom become incorporated into a collective electronic state. Here, we use resonant inelastic x-ray scattering (RIXS) on CePd$_3$ to clarify the fate of all relevant energy scales. We find that even spin-orbit excited states acquire pronounced momentum-dependence at low temperature - the telltale sign of hybridization with the underlying metallic state. Our results demonstrate how localized electronic degrees of freedom endow correlated metals with new properties, which is critical for a microscopic understanding of superconducting, electronic nematic, and topological states.

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.

Hall effect and quantum oscillation measurements on high temperature cuprate superconductors show that underdoped compositions have a small Fermi surface pocket whereas when heavily overdoped, the pocket increases dramatically in size. The origin of this change in electronic structure has been unclear, but may be related to the high temperature superconductivity. Here we show that the clean overdoped single-layer cuprate Tl2Ba2CuO6+x (Tl2201) displays CDW order with a remarkably long correlation length $\xi \approx 200$ \r{A} which disappears above a hole concentration p_CDW ~ 0.265. We show that the evolution of the electronic properties of Tl2201 as the doping is lowered may be explained by a Fermi surface reconstruction which accompanies the emergence of the CDW below p_CDW. Our results demonstrate importance of CDW correlations in understanding the electronic properties of overdoped cuprates.

In the novel stoichiometric iron-based material RbEuFe4As4 superconductivity coexists with a peculiar long-range magnetic order of Eu 4f states; their coexistance is puzzling and represents a challenge for both experiment and theory. Using angle-resolved photoemission spectroscopy, resonant photoemission spectroscopy, Andreev reflection spectroscopy and scanning tunneling spectroscopy we have addressed this puzzle and unambigously shown that Fe- and Eu-derived states are largely decoupled and that superconducting and a long range magnetic orders exist almost independently from each other., Comment: 7 pages, 8 figures, To appear in: Phys.Usp

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

In the novel stoichiometric iron-based material RbEuFe$_{4}$As$_{4}$ superconductivity coexists with a peculiar long-range magnetic order of Eu 4f states. Using angle-resolved photoemission spectroscopy, we reveal a complex three dimensional electronic structure and compare it with density functional theory calculations. Multiple superconducting gaps were measured on various sheets of the Fermi surface. High resolution resonant photoemission spectroscopy reveals magnetic order of the Eu 4f states deep into the superconducting phase. Both the absolute values and the anisotropy of the superconducting gaps are remarkably similar to the sibling compound without Eu, indicating that Eu magnetism does not affect the pairing of electrons. A complete decoupling between Fe- and Eu-derived states was established from their evolution with temperature, thus unambiguously demonstrating that superconducting and a long range magnetic orders exist independently from each other. The established electronic structure of RbEuFe$_{4}$As$_{4}$ opens opportunities for the future studies of the highly unorthodox electron pairing and phase competition in this family of iron-based superconductors with doping.

Spin-orbit interaction and structure inversion asymmetry in combination with magnetic ordering is a promising route to novel materials with highly mobile spin-polarized carriers at the surface. Spin-resolved measurements of the photoemission current from the Si-terminated surface of the antiferromagnet TbRh2Si2 and their analysis within an ab initio one-step theory unveil an unusual triple winding of the electron spin along the fourfold-symmetric constant energy contours of the surface states. A two-band k.p model is presented that yields the triple winding as a cubic Rashba effect. The curious in-plane spin-momentum locking is remarkably robust and remains intact across a paramagnetic-antiferromagnetic transition in spite of spin-orbit interaction on Rh atoms being considerably weaker than the out-of-plane exchange field due to the Tb 4f moments., Comment: 7 pages, 3 figures

A central prospect of antiferromagnetic spintronics is to exploit magnetic properties that are unavailable with ferromagnets. However, this poses the challenge of accessing such properties for readout and control. To this end, light-induced manipulation of the transient ground state, e.g. by changing the magnetic anisotropy potential, opens promising pathways towards ultrafast deterministic control of antiferromagnetism. Here, we use this approach to trigger a $\it{coherent}$ rotation of the entire long-range antiferromagnetic spin arrangement about a crystalline axis in $GdRh_2Si_2$ and demonstrate $\it{deterministic}$ control of this rotation upon ultrafast optical excitation. Our observations can be explained by a displacive excitation of the Gd spins$'$ local anisotropy potential by the optical excitation, allowing for a full description of this transient magnetic anisotropy potential.

We use resonant inelastic x-ray scattering to investigate charge-stripe correlations in La$_{1.675}$Eu$_{0.2}$Sr$_{0.125}$CuO$_4$. By differentiating elastic from inelastic scattering, it is demonstrated that charge-stripe correlations precede both the structural low-temperature tetragonal phase and the transport-defined pseudogap onset. The scattering peak amplitude from charge stripes decays approximately as $T^{-2}$ towards our detection limit. The in-plane integrated intensity, however, remains roughly temperature independent. Therefore, although the incommensurability shows a remarkably large increase at high temperature, our results are interpreted via a single scattering constituent. In fact, direct comparison to other stripe-ordered compounds (La$_{1.875}$Ba$_{0.125}$CuO$_4$, La$_{1.475}$Nd$_{0.4}$Sr$_{0.125}$CuO$_4$ and La$_{1.875}$Sr$_{0.125}$CuO$_4$) suggests a roughly constant integrated scattering intensity across all these compounds. Our results therefore provide a unifying picture for the charge-stripe ordering in La-based cuprates. As charge correlations in La$_{1.675}$Eu$_{0.2}$Sr$_{0.125}$CuO$_4$ extend beyond the low-temperature tetragonal and pseudogap phase, their emergence heralds a spontaneous symmetry breaking in this compound.

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

We present a successful synthesis method of the series Ga$_{x}$Cu$_{4-x}$(OD)$_{6}$Cl$_{2}$ with substitutions up to $x=0.8$. The compound remains a frustrated kagome system with an insulating ground state similar to herbertsmithite for these substitutions, as the additional charge of Ga$^{3+}$ is most likely bound to additional OH$^{-}$ and Cl$^{-}$. Besides infrared measurements, we present magnetic and specific-heat data down to 2 K for selected samples with $0\leq x\leq0.8$. With increasing $x$ the long-range magnetic order is suppressed, similar to what was observed in the series Zn$_{x}$Cu$_{4-x}$(OH)$_{6}$Cl$_{2}$, indicating that Ga goes predominantly to the inter-plane position of the layered crystal structure. The reduction of the frozen magnetic fraction with increasing substitution was followed by $\mu$SR measurements. $^{69,71}$Ga nuclear magnetic resonance (NMR) was applied as a local probe for Ga induced disorder. One well resolved Ga NMR line of moderate width is found for each isotope across the phase diagram which indicates a rather homogeneous distribution of the Ga isotopes on a single site in the lattice., Comment: submitted to physica status solidi

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

The notion of a simple ordered state implies homogeneity. If the order is established by a broken symmetry, elementary Landau theory of phase transitions shows that only one symmetry mode describes this state. Precisely at points of phase coexistence domain states formed of large regions of different phases can be stabilized by long range interactions. In uniaxial antiferromagnets the so-called metamagnetism is an example of such a behavior, when an antiferromagnetic and field-induced spin-polarized paramagnetic/ferromagnetic state co-exist at a jump-like transition in the magnetic phase diagram. Here, combining experiment with theoretical analysis, we show that a different type of mixed state between antiferromagnetism and ferromagnetism can be created in certain acentric materials. In the small-angle neutron scattering experiments we observe a field-driven spin-state in the layered antiferromagnet Ca3Ru2O7, which is modulated on a scale between 8 and 20 nm and has both antiferromagnetic and ferromagnetic parts. We call this state a metamagnetic texture and explain its appearance by the chiral twisting effects of the asymmetric Dzyaloshinskii-Moriya (DM) exchange. The observation can be understood as an extraordinary coexistence, in one thermodynamic state, of spin orders belonging to different symmetries. Experimentally, the complex nature of this metamagnetic state is demonstrated by measurements of anomalies in electronic transport which reflect the spin-polarization in the metamagnetic texture, determination of the magnetic orbital moments, which supports the existence of strong spin-orbit effects, a pre-requisite for the mechanism of twisted magnetic states in this material., Comment: Supplementary materials included

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.

Magnetic doping with transition metal ions is the most widely used approach to break timereversal symmetry in a topological insulator, a prerequisite for unlocking the TIs exotic potential. Recently, we reported the doping of Bi2Te3 thin films with rare earth ions, which, owing to their large magnetic moments, promise commensurately large magnetic gap openings in the topological surface states. However, only when doping with Dy has a sizable gap been observed in angle-resolved photoemission spectroscopy, which persists up to room-temperature. Although disorder alone could be ruled out as a cause of the topological phase transition, a fundamental understanding of the magnetic and electronic properties of Dy:Bi2Te3 remained elusive. Here, we present an X-ray magnetic circular dichroism, polarized neutron reflectometry, muon spin rotation, and resonant photoemission study of the microscopic magnetic and electronic properties. We find that the films are not simply paramagnetic but that instead the observed behavior can be well explained by the assumption of slowly fluctuating, inhomogeneous magnetic patches with increasing volume fraction as the temperature decreases. At liquid helium temperatures, a large effective magnetization can be easily introduced by the application of moderate magnetic fields, implying that this material is very suitable for proximity coupling to an underlying ferromagnetic insulator or in a heterostructure with transition metal-doped layers. However, the introduction of some charge carriers by the dopants cannot be excluded at least in these highly doped samples. Nevertheless, we find that the magnetic order is not mediated via the conduction channel in these rare earth doped samples and therefore magnetic order and carrier concentration are expected to be independently controllable. This is not generally the case for transition metal doped topological insulators., Comment: 9 pages, 5 figures

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

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.

We present linear polarization-dependent soft x-ray absorption spectroscopy data at the Ce $M_{4,5}$ edges of Cd and Sn doped CeCoIn$_5$. The 4$f$ ground state wave functions have been determined for their superconducting, antiferromagnetic and paramagnetic ground states. The absence of changes in the wave functions in CeCo(In$_{1-x}$Cd$_x$)$_5$ suggests the 4$f$\,--\,conduction electron ($cf$) hybridization is not affected by globally Cd doping, thus supporting the interpretation of magnetic droplets nucleating long range magnetic order. This is contrasted by changes in the wave function due to Sn substitution. Increasing Sn in CeCo(In$_{1-y}$Sn$_y$)$_5$ compresses the 4$f$ orbitals into the tetragonal plane of these materials, suggesting enhanced $cf$ hybridization with the in-plane In(1) atoms and a homogeneous altering of the electronic structure. As these experiments show, the 4$f$ wave functions are a very sensitive probe of small changes in the hybridization of 4$f$ and conduction electrons, even conveying information about direction dependencies., Comment: 6 pages, 4 figures

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

Analyzing temperature dependent photoemission (PE) data of the ferromagnetic Kondo-lattice (KL) system YbNiSn in the light of the Periodic Anderson model (PAM) we show that the KL behavior is not limited to temperatures below a temperature T_K, defined empirically from resistivity and specificic heat measurements. As characteristic for weakly hybridized Ce and Yb systems, the PE spectra reveal a 4f-derived Fermi level peak, which reflects contributions from the Kondo resonance and its crystal electric field (CEF) satellites. In YbNiSn this peak has an unusual temperature dependence: With decreasing temperature a steady linear increase of intensity is observed which extends over a large interval ranging from 100 K down to 1 K without showing any peculiarities in the region of T_K ~ TC= 5.6 K. In the light of the single-impurity Anderson model (SIAM) this intensity variation reflects a linear increase of 4f occupancy with decreasing temperature, indicating an onset of Kondo screening at temperatures above 100 K. Within the PAM this phenomenon could be described by a non-Fermi liquid like T- linear damping of the self-energy which accounts phenomenologically for the feedback from the closely spaced CEF-states., Comment: Accepted to Phys. Rev. B

The anisotropy of magnetic properties commonly is introduced in textbooks using the case of an antiferromagnetic system with Ising type anisotropy. This model presents huge anisotropic magnetization and a pronounced metamagnetic transition and is well-known and well-documented both, in experiments and theory. In contrast, the case of an antiferromagnetic $X$-$Y$ system with weak in-plane anisotropy is only poorly documented. We studied the anisotropic magnetization of the compound GdRh$_2$Si$_2$ and found that it is a perfect model system for such a weak-anisotropy setting because the Gd$^{3+}$ ions in GdRh$_2$Si$_2$ have a pure spin moment of S=7/2 which orders in a simple AFM structure with ${\bf Q} = (001)$. We observed experimentally in $M(B)$ a continuous spin-flop transition and domain effects for field applied along the $[100]$- and the $[110]$-direction, respectively. We applied a mean field model for the free energy to describe our data and combine it with an Ising chain model to account for domain effects. Our calculations reproduce the experimental data very well. In addition, we performed magnetic X-ray scattering and X-ray magnetic circular dichroism measurements, which confirm the AFM propagation vector to be ${\bf Q} = (001)$ and indicate the absence of polarization on the rhodium atoms.

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

We have performed neutron inelastic scattering and resonant inelastic X-ray scattering (RIXS) at the Cu-$L_3$ edge to study high-energy magnetic excitations at energy transfers of more than 100 meV for overdoped La$_{2-x}$Sr$_{x}$CuO$_{4}$ with $x=0.25$ ($T_c=15$ K) and $x=0.30$ (non-superconducting) using identical single crystal samples for the two techniques. From constant-energy slices of neutron scattering cross-sections, we have identified magnetic excitations up to ~250 meV for $x=0.25$. Although the width in the momentum direction is large, the peak positions along the (pi, pi) direction agree with the dispersion relation of the spin-wave in the non-doped La$_{2}$CuO$_{4}$ (LCO), which is consistent with the previous RIXS results of cuprate superconductors. Using RIXS at the Cu-$L_3$ edge, we have measured the dispersion relations of the so-called paramagnon mode along both (pi, pi) and (pi, 0) directions. Although in both directions the neutron and RIXS data connect with each other and the paramagnon along (pi, 0) agrees well with the LCO spin-wave dispersion, the paramagnon in the (pi, pi) direction probed by RIXS appears to be less dispersive and the excitation energy is lower than the spin-wave of LCO near (pi/2, pi/2). Thus, our results indicate consistency between neutron inelastic scattering and RIXS, and elucidate the entire magnetic excitation in the (pi, pi) direction by the complementary use of two probes. The polarization dependence of the RIXS profiles indicates that appreciable charge excitations exist in the same energy range of magnetic excitations, reflecting the itinerant character of the overdoped sample. A possible anisotropy in the charge excitation intensity might explain the apparent differences in the paramagnon dispersion in the (pi, pi) direction as detected by the X-ray scattering., Comment: 7 pages, 7 figures

The evolution of electronic (spin and charge) excitations upon carrier doping is an extremely important issue in superconducting layered cuprates and the knowledge of its asymmetry between electron- and hole-dopings is still fragmentary. Here we combine x-ray and neutron inelastic scattering measurements to track the doping dependence of both spin and charge excitations in electron-doped materials. Copper L3 resonant inelastic x-ray scattering spectra show that magnetic excitations shift to higher energy upon doping. Their dispersion becomes steeper near the magnetic zone center and deeply mix with charge excitations, indicating that electrons acquire a highly itinerant character in the doped metallic state. Moreover, above the magnetic excitations, an additional dispersing feature is observed near the {\Gamma}-point, and we ascribe it to particle-hole charge excitations. These properties are in stark contrast with the more localized spin-excitations (paramagnons) recently observed in hole-doped compounds even at high doping-levels., Comment: 20 pages

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 charge and spin correlations in La$_{1.875}$Ba$_{0.125}$CuO$_4$ (LBCO 1/8) are studied using Cu $L_3$ edge resonant inelastic x-ray scattering (RIXS). The static charge order (CO) is observed at a wavevector of $(0.24,0)$ and its charge nature confirmed by measuring the dependence of this peak on the incident x-ray polarization. The paramagnon excitation in LBCO 1/8 is then measured as it disperses through the CO wavevector. Within the experimental uncertainty no changes are observed in the paramagnon due to the static CO, and the paramagnon seems to be similar to that measured in other cuprates, which have no static CO. Given that the stripe correlation modulates both the charge and spin degrees of freedom, it is likely that subtle changes do occur in the paramagnon due to CO. Consequently, we propose that future RIXS measurements, realized with higher energy resolution and sensitivity, should be performed to test for these effects., Comment: 5 pages, 4 figures

One of the most intensely studied scenarios of high-temperature superconductivity (HTS) postulates pairing by exchange of magnetic excitations [1]. Indeed, such excitations have been observed up to around optimal doping in the cuprates [2-7]. In the heavily overdoped regime neutron scattering measurements indicate that magnetic excitations have effectively disappeared [8-10], and this was argued to cause the demise of HTS with overdoping [1, 8, 10]. Here we use resonant inelastic x-ray scattering (RIXS), which is sensitive to complementary parts of reciprocal space, to measure the evolution of the magnetic excitations in La2-xSrxCuO4 across the entire phase diagram, from a strongly correlated insulator (x = 0) to a non-superconducting metal (x = 0.40). For x = 0, well-defined magnon excitations are observed [11]. These magnons broaden with doping, but they persist with a similar dispersion and comparable intensity all the way to the non-superconducting, heavily overdoped metallic phase. The destruction of HTS with overdoping is therefore caused neither by the general disappearance nor by the overall softening of magnetic excitations; other factor(s), such as the redistribution of spectral weight, must be considered., Comment: See Nature Materials http://dx.doi.org/10.1038/nmat3723 for Advanced Online Publication

Many-body interactions in crystalline solids can be conveniently described in terms of quasiparticles with strongly renormalized masses as compared to those of non-interacting particles. Examples of extreme mass renormalization are on the one hand graphene, where the charge carriers obey the linear dispersion relation of massless Dirac fermions, and on the other hand heavy-fermion materials where the effective electron mass approaches the mass of a proton. Here we show that both extremes, Dirac fermions like they are found in graphene and extremely-heavy quasiparticles characteristic for Kondo materials, may not only coexist in a solid but can undergo strong mutual interactions. Using the example of EuRh2Si2 we explicitly demonstrate that these interactions can take place at the surface and in the bulk. The presence of the linear dispersion is imposed solely by the crystal symmetry while the existence of heavy quasiparticles is caused by the localized nature of the 4f states., Comment: 4 pages, 4 figures

Angle-resolved photoelectron spectroscopy, supplemented by theoretical calculations has been applied to study the electronic structure of heavy-fermion material CeFePO, a homologue to the Fe-based high-temperature superconductors, and CeFeAs_0.7P_0.3O, where the applied chemical pressure results in a ferromagnetic order of the 4f moments. A comparative analysis reveals characteristic differences in the Fe-derived band structure for these materials, implying a rather different hybridization of valence electrons to the localized 4f orbitals. In particular, our results suggest that the ferromagnetism of Ce moments in CeFeAs_0.7P_0.3O is mediated mainly by Fe 3d_xz/yz orbitals, while the Kondo screening in CeFePO is instead due to a strong interaction of Fe 3d_3z^2-r^2 orbitals., Comment: 5 pages, 3 figures, accepted for publication in Phys. Rev. B (Rapid)

We present a study of the evolution of magnetism from the quantum critical system YbRh2Si2 to the stable trivalent Yb system YbCo2Si2. Single crystals of Yb(Rh_(1-x)Co_x)2Si2 were grown for 0 < x < 1 and studied by means of magnetic susceptibility, electrical resistivity, and specific heat measurements, as well as photoemission spectroscopy. The results evidence a complex magnetic phase diagram, with a non-monotonic evolution of T_N and two successive transitions for some compositions resulting in two tricritical points. The strong similarity with the phase diagram of YbRh2Si2 under pressure indicates that Co substitution basically corresponds to the application of positive chemical pressure. Analysis of the data proves a strong reduction of the Kondo temperature T_K with increasing Co content, T_K becoming smaller than T_N for x ~ 0.5, implying a strong localization of the 4f electrons. Furthermore, low-temperature susceptibility data confirm a competition between ferromagnetic and antiferromagnetic exchange. The series Yb(Rh_(1-x)Co_x)2Si2 provides an excellent experimental opportunity to gain a deeper understanding of the magnetism at the quantum critical point in the vicinity of YbRh2Si2 where the antiferromagnetic phase disappears (T_N=>0)., Comment: 11 pages, 9 figures

Being homologue to the new, Fe-based type of high-temperature superconductors, CeFePO exhibits magnetism, Kondo and heavy-fermion phenomena. We experimentally studied the electronic structure of CeFePO by means of angle-resolved photoemission spectroscopy. In particular, contributions of the Ce 4f-derived states and their hybridization to the Fe 3d bands were explored using both symmetry selection rules for excitation and their photoionization cross-section variations as a function of photon energy. It was experimentally found - and later on confirmed by LDA as well as DMFT calculations - that the Ce 4f states hybridize to the Fe 3d states of d_{3z^2-r^2} symmetry near the Fermi level that discloses their participation in the occurring electron-correlation phenomena and provides insight into mechanism of superconductivity in oxopnictides., Comment: 5 pages, 3 figures