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We report a neutron spin-echo study of the critical dynamics in the S=52 antiferromagnets MnF2 and Rb2MnF4 with three-dimensional (3D) and two-dimensional (2D) spin systems, respectively, in zero external field. Both compounds are Heisenberg antiferromagnets with a small uniaxial anisotropy resulting from dipolar spin-spin interactions, which leads to a crossover in the critical dynamics close to the Néel temperature, TN. By taking advantage of the μeV energy resolution of the spin-echo spectrometer, we have determined the dynamical critical exponents z for both longitudinal and transverse fluctuations. In MnF2, both the characteristic temperature for crossover from 3D Heisenberg to 3D Ising behavior and the exponents z in both regimes are consistent with predictions from the dynamical scaling theory. The amplitude ratio of longitudinal and transverse fluctuations also agrees with predictions. In Rb2MnF4, the critical dynamics crosses over from the expected 2D Heisenberg behavior for T TN to a scaling regime with exponent z=1.387(4), which has not been predicted by theory and may indicate the influence of long-range dipolar interactions.

We present here a newly developed software tool (called PGMweb) for computing and simulating the X-ray beam path through a plane grating monochromator (PGM), a key component in soft X-ray beamlines at modern synchrotron and free-electron laser facilities. A historical overview of the development of PGMs is presented, with special attention dedicated to the collimated PGM optical scheme found at several X-ray facilities worldwide. The analytical expressions that fully describe the geometry of a PGM are derived and have been implemented as functions in a Python library (pyplanemono). PGMweb is distributed as a web-based application that can be run in any modern browser without installation, making its use very straightforward for X-ray beamline designers and beamline scientists alike., (open access.)

Resonant inelastic x-ray scattering (RIXS) using an incident energy tuned to the uraniumN4,5absorption edges is reported from epitaxial films of α -U 3 O 8 and UN. Theory shows that for U 3 O 8 the multiplets associated with a 5 f 1 configuration with a ground state of2F5/2and the excited state of2F7/2are observed. However, the strong transition predicted at a transfer energy of 1.67 eV is not observed. We assume this is a consequence of the intermediate state lifetime broadening due to interaction with continuum states when the transferred energy exceeds the onset of the continuum in the presence of the core hole. This hypothesis is supported by the results obtained for the 5 f -itinerant system UN, where no sharp transitions have been observed, although the broad scattering response centred at ∼1 eV is considered a signature of a predominantly 5 f 3 configuration in this band-like semi-metallic system. These experiments and theory add important information on these materials, both of which have been investigated since the 1960s, as well as whether RIXS at the uranium N edge can become a valuable tool for actinide research., (© 2023 IOP Publishing Ltd.)

Among condensed matter systems, Mott insulators exhibit diverse properties that emerge from electronic correlations. In itinerant metals, correlations are usually weak, but can also be enhanced via geometrical confinement of electrons, that manifest as 'flat' dispersionless electronic bands. In the fast developing field of topological materials, which includes Dirac and Weyl semimetals, flat bands are one of the important components that can result in unusual magnetic and transport behaviour. To date, characterisation of flat bands and their magnetism is scarce, hindering the design of novel materials. Here, we investigate the ferromagnetic Kagomé semimetal Co 3 Sn 2 S 2 using resonant inelastic X-ray scattering. Remarkably, nearly non-dispersive Stoner spin excitation peaks are observed, sharply contrasting with the featureless Stoner continuum expected in conventional ferromagnetic metals. Our band structure and dynamic spin susceptibility calculations, and thermal evolution of the excitations, confirm the nearly non-dispersive Stoner excitations as unique signatures of correlations and spin-polarized electronic flat bands in Co 3 Sn 2 S 2 . These observations serve as a cornerstone for further exploration of band-induced symmetry-breaking orders in topological materials., (© 2022. The Author(s).)

The microscopic origins of emergent behaviours in condensed matter systems are encoded in their excitations. In ordinary magnetic materials, single spin-flips give rise to collective dipolar magnetic excitations called magnons. Likewise, multiple spin-flips can give rise to multipolar magnetic excitations in magnetic materials with spin S ≥ 1. Unfortunately, since most experimental probes are governed by dipolar selection rules, collective multipolar excitations have generally remained elusive. For instance, only dipolar magnetic excitations have been observed in isotropic S = 1 Haldane spin systems. Here, we unveil a hidden quadrupolar constituent of the spin dynamics in antiferromagnetic S = 1 Haldane chain material Y 2 BaNiO 5 using Ni L 3 -edge resonant inelastic x-ray scattering. Our results demonstrate that pure quadrupolar magnetic excitations can be probed without direct interactions with dipolar excitations or anisotropic perturbations. Originating from on-site double spin-flip processes, the quadrupolar magnetic excitations in Y 2 BaNiO 5 show a remarkable dual nature of collective dispersion. While one component propagates as non-interacting entities, the other behaves as a bound quadrupolar magnetic wave. This result highlights the rich and largely unexplored physics of higher-order magnetic excitations., (© 2022. The Author(s).)

Since the discovery of charge disproportionation in the FeO_{2} square-lattice compound Sr_{3}Fe_{2}O_{7} by Mössbauer spectroscopy more than fifty years ago, the spatial ordering pattern of the disproportionated charges has remained "hidden" to conventional diffraction probes, despite numerous x-ray and neutron scattering studies. We have used neutron Larmor diffraction and Fe K-edge resonant x-ray scattering to demonstrate checkerboard charge order in the FeO_{2} planes that vanishes at a sharp second-order phase transition upon heating above 332 K. Stacking disorder of the checkerboard pattern due to frustrated interlayer interactions broadens the corresponding superstructure reflections and greatly reduces their amplitude, thus explaining the difficulty of detecting them by conventional probes. We discuss the implications of these findings for research on "hidden order" in other materials.

In ultrathin films of FeSe grown on SrTiO 3 (FeSe/STO), the superconducting transition temperature T c is increased by almost an order of magnitude, raising questions on the pairing mechanism. As in other superconductors, antiferromagnetic spin fluctuations have been proposed to mediate SC making it essential to study the evolution of the spin dynamics of FeSe from the bulk to the ultrathin limit. Here, we investigate the spin excitations in bulk and monolayer FeSe/STO using resonant inelastic x-ray scattering (RIXS) and quantum Monte Carlo (QMC) calculations. Despite the absence of long-range magnetic order, bulk FeSe displays dispersive magnetic excitations reminiscent of other Fe-pnictides. Conversely, the spin excitations in FeSe/STO are gapped, dispersionless, and significantly hardened relative to its bulk counterpart. By comparing our RIXS results with simulations of a bilayer Hubbard model, we connect the evolution of the spin excitations to the Fermiology of the two systems revealing a remarkable reconfiguration of spin excitations in FeSe/STO, essential to understand the role of spin fluctuations in the pairing mechanism.

We explore the existence of the collective orbital excitations, orbitons, in the canonical orbital system KCuF_{3} using the Cu L_{3}-edge resonant inelastic x-ray scattering. We show that the nondispersive high-energy peaks result from the Cu^{2+}  dd orbital excitations. These high-energy modes display good agreement with the ab initio quantum chemistry calculation, indicating that the dd excitations are highly localized. At the same time, the low-energy excitations present clear dispersion. They match extremely well with the two-spinon continuum following the comparison with Müller ansatz calculations. The localized dd excitations and the observation of the strongly dispersive magnetic excitations suggest that the orbiton dispersion is below the resolution detection limit. Our results can reconcile with the strong local Jahn-Teller effect in KCuF_{3}, which predominantly drives orbital ordering.

The discovery of superconductivity in a d^{9-δ} nickelate has inspired disparate theoretical perspectives regarding the essential physics of this class of materials. A key issue is the magnitude of the magnetic superexchange, which relates to whether cuprate-like high-temperature nickelate superconductivity could be realized. We address this question using Ni L-edge and O K-edge spectroscopy of the reduced d^{9-1/3} trilayer nickelates R_{4}Ni_{3}O_{8} (where R=La, Pr) and associated theoretical modeling. A magnon energy scale of ∼80  meV resulting from a nearest-neighbor magnetic exchange of J=69(4)  meV is observed, proving that d^{9-δ} nickelates can host a large superexchange. This value, along with that of the Ni-O hybridization estimated from our O K-edge data, implies that trilayer nickelates represent an intermediate case between the infinite-layer nickelates and the cuprates. Layered nickelates thus provide a route to testing the relevance of superexchange to nickelate superconductivity.

Resonant inelastic x-ray spectroscopy at the uranium N 4 absorption edge at 778 eV has been used to reveal the excitations in UO 2 up to 1 eV. The earlier (1989) studies by neutron inelastic scattering of the crystal-field states within the 3 H 4 multiplet are confirmed. In addition, the first excited state of the 3 F 2 multiplet at ∼520 meV has been established, and there is a weak signal corresponding to the next excited state at ∼920 meV. This represents a successful application of soft x-ray spectroscopy to an actinide sample, and resolves an open question in UO 2 that has been discussed for 50 years. The technique is described and important caveats are drawn about possible future applications.

High T_{c} superconductors show a rich variety of phases associated with their charge degrees of freedom. Valence charges can give rise to charge ordering or acoustic plasmons in these layered cuprate superconductors. While charge ordering has been observed for both hole- and electron-doped cuprates, acoustic plasmons have only been found in electron-doped materials. Here, we use resonant inelastic x-ray scattering to observe the presence of acoustic plasmons in two families of hole-doped cuprate superconductors (La_{1.84}Sr_{0.16}CuO_{4} and Bi_{2}Sr_{1.6}La_{0.4}CuO_{6+δ}), crucially completing the picture. Interestingly, in contrast to the quasistatic charge ordering which manifests at both Cu and O sites, the observed acoustic plasmons are predominantly associated with the O sites, revealing a unique dichotomy in the behavior of valence charges in hole-doped cuprates.

The discovery of charge-density-wave-related effects in the resonant inelastic x-ray scattering spectra of cuprates holds the tantalizing promise of clarifying the interactions that stabilize the electronic order. Here, we report a comprehensive resonant inelastic x-ray scattering study of La_{2-x}Sr_{x}CuO_{4} finding that charge-density wave effects persist up to a remarkably high doping level of x=0.21 before disappearing at x=0.25. The inelastic excitation spectra remain essentially unchanged with doping despite crossing a topological transition in the Fermi surface. This indicates that the spectra contain little or no direct coupling to electronic excitations near the Fermi surface, rather they are dominated by the resonant cross section for phonons and charge-density-wave-induced phonon softening. We interpret our results in terms of a charge-density wave that is generated by strong correlations and a phonon response that is driven by the charge-density-wave-induced modification of the lattice.

Understanding many-body physics of elementary excitations has advanced our control over material properties. Here, we study spin-flip excitations in NiO using Ni L_{3}-edge resonant inelastic x-ray scattering (RIXS) and present a strikingly different resonant energy behavior between single and double spin-flip excitations. Comparing our results with single-site full-multiplet ligand field theory calculations we find that the spectral weight of the double-magnon excitations originates primarily from the double spin-flip transition of the quadrupolar RIXS process within a single magnetic site. Quadrupolar spin-flip processes are among the least studied excitations, despite being important for multiferroic or spin-nematic materials due to their difficult detection. We identify intermediate state multiplets and intra-atomic core-valence exchange interactions as the key many-body factors determining the fate of such excitations. RIXS resonant energy dependence can act as a convincing proof of existence of nondipolar higher-ranked magnetic orders in systems for which, only theoretical predictions are available.

X-ray diffraction, specific heat, magnetic susceptibility and inelastic x-ray scattering measurements on the transurarium oxypnictides NpFeAsO and NpFeAsO0.85F0.15 are presented. No superconductivity down to 2 K was observed upon fluorine doping, contrary to the structurally analogous rare-earth pnictides. No modification of the phonon density of states was observed upon doping with fluorine. We discuss our results in light of the latest experimental and theoretical studies on the role of phonons in the superconducting pnictide compounds.

We report a neutron scattering study of the magnetic order and dynamics of the bilayer perovskite Sr(3)Fe(2)O(7), which exhibits a temperature-driven metal-insulator transition at 340 K. We show that the Fe(4+) moments adopt incommensurate spiral order below T(N) = 115 K and provide a comprehensive description of the corresponding spin-wave excitations. The observed magnetic order and excitation spectra can be well understood in terms of an effective spin Hamiltonian with interactions ranging up to third-nearest-neighbor pairs. The results indicate that the helical magnetism in Sr(3)Fe(2)O(7) results from competition between ferromagnetic double-exchange and antiferromagnetic superexchange interactions whose strengths become comparable near the metal-insulator transition. They thus confirm a decades-old theoretical prediction and provide a firm experimental basis for models of magnetic correlations in strongly correlated metals.

We present the first angle-resolved photoemission studies of electronic structure in CaC6, a superconducting graphite intercalation compound with T_{c}=11.6 K. We find that, contrary to theoretical models, the electron-phonon coupling on the graphene-derived Fermi sheets with high-frequency graphene-derived phonons is surprisingly strong and anisotropic. The shape of the Fermi surface is found to favor a dynamical intervalley nesting via exchange of high-frequency phonons. Our results suggest that graphene sheets play a crucial role in superconductivity in graphite intercalation compounds.