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We examine the influence at room temperature of the deposit of a water layer on the phonon dynamics of a solid. It is shown that the water wetting at the surface of an Alumina monocrystal has deep effects on acoustic phonons, propagating over several hundred microns distance and taking place on a relatively long time scale. The effect of the wetting at the boundary is two-fold: a hardening of both transverse and longitudinal acoustic phonons is observed as well as a relaxation of internal stresses. These acoustic phonon energy changes were observed by inelastic X-ray scattering up to 40 meV energy loss, allowing us to probe the solid at different depths from the surface.

We use diffuse and inelastic x-ray scattering to study the formation of an incommensurate charge-density-wave (I-CDW) in BaNi$_2$As$_2$, a candidate system for charge-driven electronic nematicity. Intense diffuse scattering is observed around the modulation vector of the I-CDW, $Q_{I-CDW}$. It is already visible at room temperature and collapses into superstructure reflections in the long-range ordered state where a small orthorhombic distortion occurs. A clear dip in the dispersion of a low-energy transverse optical phonon mode is observed around $Q_{I-CDW}$. The phonon continuously softens upon cooling, ultimately driving the transition to the I-CDW state. The transverse character of the soft-phonon branch elucidates the complex pattern of the I-CDW satellites observed in the current and earlier studies and settles the debated unidirectional nature of the I-CDW. The phonon instability and its reciprocal space position is well captured by our ${ab}$ ${initio}$ calculations. These however indicate that neither Fermi surface nesting, nor enhanced momentum-dependent electron-phonon coupling can account for the I-CDW formation, demonstrating its unconventional nature.% and suggest alternative origins of the I-CDW., Comment: Revised version - to appear in PRL

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.

Understanding the role of disorder and the correlations that exist within it, is one of the defining challenges in contemporary materials science. However, there are few material systems, devoid of other complex interactions, which can be used to systematically study the effects of crystallographic conflict on correlated disorder. Here, we report extensive diffuse x-ray scattering studies on the epitaxially stabilised alloy $\mbox{U}_{1-x}\mbox{Mo}_x$, showing that a new form of intrinsically tuneable correlated disorder arises from a mismatch between the preferred symmetry of a crystallographic basis and the lattice upon which it is arranged. Furthermore, combining grazing incidence inelastic x-ray scattering and state-of-the-art ab initio molecular dynamics simulations we discover strong disorder-phonon coupling. This breaks global symmetry and dramatically suppresses phonon-lifetimes compared to alloying alone, providing an additional design strategy for phonon engineering. These findings have implications wherever crystallographic conflict can be accommodated and may be exploited in the development of future functional materials., Comment: V3: Some supplementary content moved into main text and manuscript structure reformatted to accommodate. No substantive change to transferred material but linking statements added. Section III discussion expanded by one paragraph. No change to results, figures, or conclusions in either the main manuscript or supplementary material. Main text: 10 pg, 7 figs. SM: 14 pg, 5 figs, 1 table

We report experiments to determine the effect of radiation damage on the phonon spectra of the most common nuclear fuel, UO$_2$. We have irradiated thin ($\sim$ 300 nm) epitaxial films of UO$_2$ with 2.1 MeV He$^{2+}$ ions to 0.15 dpa and a lattice swelling of $\Delta$a/a $\sim$ 0.6 %, and then used grazing-incidence inelastic X-ray scattering to measure the phonon spectrum. We succeeded to observe the acoustic modes, both transverse and longitudinal, across the Brillouin zone. The phonon energies, in both the pristine and irradiated samples, are unchanged from those observed in bulk material. On the other hand, the phonon linewidths (inversely proportional to the phonon lifetimes), show a significant broadening when comparing the pristine and irradiated samples. This effect is shown to increase with phonon energy across the Brillouin zone. The decreases in the phonon lifetimes of the acoustic modes are roughly consistent with a 50 % reduction in the thermal conductivity., Comment: 11 pages, 7 figures

In the spinel compound GeCo$_2$O$_4$, the Co$^{2+}$ pyrochlore sublattice presents remarkable magnetic field-induced behaviors that we unveil through neutron and X-ray single-crystal diffraction. The N\'eel ordered magnetic phase is entered through a structural lowering of the cubic symmetry. In this phase, when a magnetic field is applied along a 2-fold cubic direction, a spin-flop transition of one fourth of the magnetic moments releases the magnetic frustration and triggers magnetostructural effects. At high field, these ultimately lead to an unusual spin reorientation associated to structural changes.

We report an experimental and theoretical investigation of the lattice dynamics and thermal properties of the actinide dioxide NpO$_2$. The energy-wavevector dispersion relation for normal modes of vibration propagating along the $[001]$, $[110]$, and $[111]$ high-symmetry lines in NpO$_2$ at room temperature has been determined by measuring the coherent one-phonon scattering of X-rays from a $\sim$1.2 mg single-crystal specimen, the largest available single crystal for this compound. The results are compared against ab initio phonon dispersions computed within the first-principles density functional theory in the generalized gradient approximation plus Hubbard $U$ correlation (GGA+$U$) approach, taking into account third-order anharmonicity effects in the quasiharmonic approximation. Good agreement with the experiment is obtained for calculations with an on-site Coulomb parameter $U = 4$ eV and Hund's exchange $J= 0.6$ eV in line with previous electronic structure calculations. We further compute the thermal expansion, heat capacity, thermal conductivity, phonon linewidth, and thermal phonon softening, and compare with available experiments. The theoretical and measured heat capacities are in close agreement with another. About 27% of the calculated thermal conductivity is due to phonons with energy higher than 25 meV ($\sim$ 6 THz ), suggesting an important role of high-energy optical phonons in the heat transport. The simulated thermal expansion reproduces well the experimental data up to about 1000 K, indicating a failure of the quasiharmonic approximation above this limit., Comment: 12 pages, 10 figures

The magnetic excitation spectrum in the bilayer iridate Sr$_3$Ir$_2$O$_7$ has been investigated using high-resolution resonant inelastic x-ray scattering (RIXS) performed at the iridium L$_3$ edge and theoretical techniques. A study of the systematic dependence of the RIXS spectrum on the orientation of the wavevector transfer, $\mathbf{Q}$, with respect to the iridium-oxide bilayer has revealed that the magnon dispersion is comprised of two branches well separated in energy and gapped across the entire Brillouin zone. Our results contrast with those of an earlier study which reported the existence of a single dominant branch. While these earlier results were interpreted as two overlapping modes within a spin-wave model of weakly coupled iridium-oxide planes, our results are more reminiscent of those expected for a system of weakly coupled dimers. In this latter approach the lower and higher energy modes find a natural explanation as those corresponding to transverse and longitudinal fluctuations, respectively. We have therefore developed a bond-operator theory which describes the magnetic dispersion in Sr$_3$Ir$_2$O$_7$ in terms of quantum dimer excitations. In our model dimerisation is produced by the leading Heisenberg exchange, $J_c$, which couples iridium ions in adjacent planes of the bilayer. The Hamiltonian also includes in plane exchange, $J$, as well as further neighbour couplings and relevant anisotropies. The bond-operator theory provides an excellent account of the dispersion of both modes, while the measured $\mathbf{Q}$ dependence of the RIXS intensities is in reasonable qualitative accord with the spin-spin correlation function calculated from the theory. We discuss our results in the context of the quantum criticality of bilayer dimer systems in the presence of anisotropic interactions derived from strong spin-orbit coupling., Comment: 9 pages, 6 figures

We present a study of the magnetic and crystallographic structure of TbMnO$_3$ in the presence of crossed electric and magnetic fields using circularly polarised X-ray non-resonant scattering. A comprehensive account is presented of the scattering theory and data analysis methods used in our earlier studies, and in addition we present new high magnetic field data and its analysis. We discuss in detail how polarisation analysis was used to reveal structural information, including the arrangement of Tb moments which we proposed for $H = 0$ T, and how the diffraction data for $H H_C$ as for $H < H_C$. Finally some observations regarding the kinetics and the conservation of domain population at the transition are described., Comment: 14 pages, 9 figures, accepted for publication in Phys. Rev. B

Pressure is the cleanest way to tune heavy fermion systems to a quantum phase transition in order to study the rich physics and competing phases, and the comparison between ytterbium and cerium systems is particularly fruitful. We briefly review the mechanisms in play and show some examples of expected and unexpected behaviour. We emphasize the importance of the valence changes under pressure and show how modern synchrotron techniques can accurately determine this, including at low temperature., Comment: To appear in proceedings of International Conference on Superconductivity and Magnetism ICSM 2012 (Istanbul)

Magneto-electric multiferroics exemplified by TbMnO3 possess both magnetic and ferroelectric long-range order. The magnetic order is mostly understood, whereas the nature of the ferroelectricity has remained more elusive. Competing models proposed to explain the ferroelectricity are associated respectively with charge transfer and ionic displacements. Exploiting the magneto-electric coupling, we use an electric field to produce a single magnetic domain state, and a magnetic field to induce ionic displacements. Under these conditions, interference charge-magnetic X-ray scattering arises, encoding the amplitude and phase of the displacements. When combined with a theoretical analysis, our data allow us to resolve the ionic displacements at the femtoscale, and show that such displacements make a significant contribution to the zero-field ferroelectric moment., Comment: This is the author's version of the work. It is posted here by permission of the AAAS for personal use, not for redistribution. The definitive version was published in Science VOL 333, (2011), doi:10.1126/science.1208085

The magnetic structures adopted by the Fe and Sm sublattices in SmFeAsO have been investigated using element specific x-ray resonant and non-resonant magnetic scattering techniques. Between 110 and 5 K, the Sm and Fe moments are aligned along the c and a directions, respectively according to the same magnetic representation $\Gamma_{5}$ and the same propagation vector (1, 0, 0.5). Below 5 K, magnetic order of both sublattices change to a different magnetic structure and the Sm moments reorder in a magnetic unit cell equal to the chemical unit cell. Modeling of the temperature dependence for the Sm sublattice as well as a change in the magnetic structure below 5 K provide a clear evidence of a surprisingly strong coupling between the two sublattices, and indicate the need to include anisotropic exchange interactions in models of SmFeAsO and related compounds., Comment: 8 pages, 7 figures, accepted for publication in Phys. Rev. B

The magnetic structure of multiferroic Ni$_3$V$_2$O$_8$ has been investigated using non-resonant X-ray magnetic scattering. Incident circularly polarized X-rays combined with full polarization analysis of the scattered beam is shown to yield high sensitivity to the components of the cycloidal magnetic order, including their relative phases. New information on the magnetic structure in the ferroelectric phase is obtained, where it is found that the magnetic moments on the "cross-tie" sites are quenched relative to those on the "spine" sites. This implies that the onset of ferroelectricity is associated mainly with spine site magnetic order. We also demonstrate that our technique enables the imaging of multiferroic domains through polarization enhanced topography. This approach is used to image the domains as the sample is cycled by an electric field through its hysteresis loop, revealing the gradual switching of domains without nucleation., Comment: 9 pages, 6 figures

Low temperature magnetic properties of Cd-doped Ce2MIn8 (M = Rh and Ir) single crystals are investigated. Experiments of temperature dependent magnetic susceptibility, heat capacity and electrical resistivity measurements revealed that Cd-doping enhances the antiferromagnetic (AFM) ordering temperature from TN = 2.8 K (x = 0) to TN = 4.8 K (x = 0.21) for Ce2RhIn8-xCdx and induces long range AFM ordering with TN = 3.8 K (x = 0.21) for Ce2IrIn8-xCdx. Additionally, X-ray and neutron magnetic scattering studies showed that Cd-doped samples present below TN a commensurate antiferromagnetic structure with a propagation vector (1/2,1/2,0). The resolved magnetic structures for both compounds indicate that the Cd-doping tends to rotate the direction of the ordered magnetic moments toward the ab-plane. This result suggests that the Cd-doping affects the Ce3+ ground state single ion anisotropy modifying the crystalline electrical field (CEF) parameters at the Ce3+ site. Indications of CEF evolution induced by Cd-doping were also found in the electrical resistivity measurements. Comparisons between our results and the general effects of Cd-doping on the related compounds CeMIn5 (M = Co, Rh and Ir) confirms the claims that the Cd-doping induced electronic tuning is the main effect favoring AFM ordering in these compounds.

We have investigated the antiferromagnetic insulating phase of the Mott-Hubbard insulator V$_2$O$_3$ by resonant x-ray Bragg diffraction at the vanadium K-edge. Combining the information obtained from azimuthal angle scans, linear incoming polarization scans and by fitting collected data to the scattering amplitude derived from the established chemical I2/a and magnetic space groups we provide evidence of the ordering motif of anapolar moments (which results from parity violation coupling to an electromagnetic field). Experimental data (azimuthal dependence and polarization analysis) collected at space-group forbidden Bragg reflections are successfully accounted within our model in terms of vanadium magnetoelectric multipoles. We demonstrate that resonant x-ray diffraction intensities in all space-group forbidden Bragg reflections of the kind $(hkl)_m$ with odd $h$ are produced by an E1-E2 event. The determined tensorial parameters offer a test for ab-initio calculations in this material, that can lead to a deeper and more quantitative understanding of the physical properties of V$_2$O$_3$.

Non-resonant X-ray magnetic scattering has been used to study the magnetic structure of multiferroic TbMnO3 in its ferroelectric phase. Circularly polarized X-rays were combined with a full polarization analysis of the scattered beam to reveal important new information on the magnetic structure of this canonical multiferroic. An applied electric field is shown to create a magnetic nearly mono-domain state in which the cylcoidal order on the Mn sublattice rotates either clockwise or counter-clockwise depending on the sign of the field. It is demonstrated how this technique provides sensitivity to the absolute sense of rotation of the Mn moments, and to components of the ordering on the Tb sublattice and phase shifts that earlier neutron diffraction experiments could not resolve., Comment: 4 pages, 3 figures

We report on an extensive investigation of the multiferroic compound TbMnO$_3$. Non-resonant x-ray magnetic scattering (NRXMS) revealed a dominant $A$-type domain. The temperature dependence of the intensity and wavevector associated with the incommensurate magnetic order was found to be in good agreement with neutron scattering data. XRS experiments were performed in the vicinity of the Mn $K$ and Tb $L_3$ edges in the high-temperature collinear phase, the intermediate temperature cycloidal/ferroelectric phase, and the low-temperature phase. In the collinear phase resonant $E1-E1$ satellites were found at the Mn $K$ edge associated with $A$-type but also $F$-type peaks. The azimuthal dependence of the $F$-type satellites (and their absence in the NRXMS experiments) indicates that they are most likely non-magnetic in origin. We suggest instead that they may be associated with an induced charge multipole. At the Tb $L_3$ edge resonant $A$- and $F$-type satellites ($E1-E1$) were observed in the collinear phase. These we attribute to a polarisation of the Tb 5$d$ states by the ordering of the Mn sublattice. In the cycloidal/ferroelectric phase a new set of resonant satellites appear corresponding to $C$-type order. These appear at the Tb $L_3$ edge only. In addition to a dominant $E1-E1$ component in the $\sigma-\pi^\prime$ channel, a weaker component is found in the pre-edge with $\sigma-\sigma^\prime$ polarization. Calculations of the XRS were performed using the $FDMNES$ code showing that the unrotated $\sigma-\sigma^\prime$ component of the Tb $L_3$ $C$-type peaks appearing in the ferroelectric phase contains a contribution from a multipole that is odd with respect to both space and time, known in various contexts as the anapole., Comment: Phys. Rev. B (In press)

The magnetic structure of the intermetallic antiferromagnet Sm2IrIn8 was determined using x-ray resonant magnetic scattering (XRMS). Below TN = 14.2, Sm2IrIn8 has a commensurate antiferromagnetic structure with a propagation vector (1/2,0,0). The Sm magnetic moments lie in the ab plane and are rotated roughly 18 degrees away from the a axis. The magnetic structure of this compound was obtained by measuring the strong dipolar resonant peak whose enhancement was of over two orders of magnitude at the L2 edge. At the L3 edge both quadrupolar and dipolar features were observed in the energy line shape. The magnetic structure and properties of Sm2IrIn8 are found to be consistent with the general trend already seen for the Nd-, Tb- and the Ce-based compounds from the RmMnIn3m+2n family (R = rare earth; M=Rh or Ir, m = 1, 2; n = 0, 1), where the crystalline electrical field (CEF) effects determine the direction of magnetic moments and the TN evolution in the series. The measured Neel temperature for Sm2IrIn8 is slightly suppressed when compared to the TN of the parent cubic compound SmIn3., Comment: 09 pages, 06 figures, Submitted to Phys. Rev. B

Complete polarization analysis applied to resonant x-ray scattering at the Cr K-edge in K2CrO4 shows that incident linearly polarized x-rays can be converted into circularly polarized x-rays by diffraction at the Cr pre-edge (E = 5994 eV). The physical mechanism behind this phenomenon is a subtle interference effect between purely dipole (E1-E1) and purely quadrupole (E2-E2) transitions, leading to a phase shift between the respective scattering amplitudes. This effect may be exploited to disentangle two close-lying resonances that appear as a single peak in a conventional energy scan, in this way allowing to single out and identify the different multipole order parameters involved., Comment: 6 pages, 6 figures

We performed near-edge x-ray absorption spectroscopy (XANES) at V K edge in the antiferromagnetic insulating (AFI) phase of a 2.8% Cr-doped V_2O_3 single crystal. Linear dichroism of several percent is measured in the hexagonal plane and found to be in good agreement with ab-initio calculations based on multiple scattering theory. This experiment definitively proves the structural origin of the signal and therefore solves a controversy raised by previous interpretations of the same dichroism as non-reciprocal. It also calls for a further investigation of the role of the magnetoelectric annealing procedure in cooling to the AFI phase., Comment: 4 pages 3 figures. To be published in Phys. Rev. B (2005)

A thorough tensor analysis of the Bragg-forbidden reflection (00.3)$_h$ in corundum systems having a global center of inversion, like V$_2$O$_3$ and $\alpha$-Fe$_2$O$_3$, shows that anomalous x-ray resonant diffraction can access chiral properties related to the dipole-quadrupole (E1-E2) channel via an interference with the pure quadrupole-quadrupole (E2-E2) process. This is also confirmed by independent {\it ab initio} numerical simulations. In such a way it becomes possible, in this particular case, to estimate the intensity of the ``twisted'' trigonal crystal field ($C_3$ symmetry) and, in general, to detect chiral quantities in systems where dichroic absorption techniques are ineffective., Comment: 4 pages, 4 figures