RESUMEN

A compact spectrometer for medium-resolution resonant and non-resonant X-ray emission spectroscopy in von Hámos geometry is described. The main motivation for the design and construction of the spectrometer is to allow for acquisition of non-resonant X-ray emission spectra while measuring non-resonant X-ray Raman scattering spectra at beamline ID20 of the European Synchrotron Radiation Facility. Technical details are provided and the performance and possible use of the spectrometer are demonstrated by presenting results of several X-ray spectroscopic methods on various compounds.

RESUMEN

An end-station for resonant inelastic X-ray scattering and (resonant) X-ray emission spectroscopy at beamline ID20 of ESRF - The European Synchrotron is presented. The spectrometer hosts five crystal analysers in Rowland geometry for large solid angle collection and is mounted on a rotatable arm for scattering in both the horizontal and vertical planes. The spectrometer is optimized for high-energy-resolution applications, including partial fluorescence yield or high-energy-resolution fluorescence detected X-ray absorption spectroscopy and the study of elementary electronic excitations in solids. In addition, it can be used for non-resonant inelastic X-ray scattering measurements of valence electron excitations.

RESUMEN

An end-station for X-ray Raman scattering spectroscopy at beamline ID20 of the European Synchrotron Radiation Facility is described. This end-station is dedicated to the study of shallow core electronic excitations using non-resonant inelastic X-ray scattering. The spectrometer has 72 spherically bent analyzer crystals arranged in six modular groups of 12 analyzer crystals each for a combined maximum flexibility and large solid angle of detection. Each of the six analyzer modules houses one pixelated area detector allowing for X-ray Raman scattering based imaging and efficient separation of the desired signal from the sample and spurious scattering from the often used complicated sample environments. This new end-station provides an unprecedented instrument for X-ray Raman scattering, which is a spectroscopic tool of great interest for the study of low-energy X-ray absorption spectra in materials under in situ conditions, such as in operando batteries and fuel cells, in situ catalytic reactions, and extreme pressure and temperature conditions.

RESUMEN

We report a study on the temperature dependence of charge-neutral crystal field (dd) excitations in cupric oxide, using nonresonant inelastic x-ray scattering spectroscopy. Thanks to a very high-energy resolution (ΔE = 60 meV), we observe thermal effects on the dd excitation spectrum fine structure between temperatures of 10-320 K. The spectra broaden considerably with increasing temperature, consistently with an enhancement of the coupling between crystal field excitations and the temperature-dependent continuum of states above the band gap. We discuss this and other mechanisms that may explain this temperature dependence.

RESUMEN

The high frequency dynamics of liquid iodine has been investigated by deep inelastic x-ray scattering at exchanged wave-vectors (q) ranging from 2.5 to 15 Å(-1). The experimental data have been analyzed in the frame of the Sachs-Teller theory of the molecular spectrum while accounting for final state corrections to the lineshape. The performed data analysis carries insights on physical quantities as relevant as the mean rototranslational kinetic energy and the mean square Laplacian of the intermolecular potential. In both cases the measured values are consistent with corresponding theoretical expectations.

RESUMEN

We measured the dynamic structure factor of the liquid and glassy phases of the LiCl-6H(2)O solution by means of inelastic scattering of radiation in the visible, UV, and x-ray range, between 1 GHz and 10 THz, and by means of photon-correlation spectroscopy, between 0.01 Hz and 20 kHz. The measurements were performed in the temperature range between 353 and 80 K. Our data show that a single-relaxation process exists at high temperature, which has features similar to those of the single relaxation of pure water. Upon cooling the system below approximately 220 K, this single mode starts to differentiate two processes, a structural (alpha-) and a secondary (beta-) relaxation. As the temperature is decreased, the beta-relaxation is the vanishing continuation of the single, high-temperature process, while the onset of the alpha-relaxation occurs at the expense of the beta-process.

RESUMEN

Inelastic x-ray scattering has been utilized to study the elementary excitations of normal liquid 3He at the temperature T=1.10+/-0.05 K and saturated vapor pressure in the wave vector range 0.15

RESUMEN

We have studied by inelastic x-ray scattering, at wave vectors 1 nm < or =q< or =15 nm(-1), the high-frequency dynamics of epoxy-amine mixtures as the monomers irreversibly polymerize. We find that chemical bonding, while inducing molecular ordering on a mesoscopic length scale, also efficiently realizes the mechanism of dynamical arrest described by the mode-coupling theory, as manifested by a cusp singularity in the behavior of the nonergodicity factor as a function of the number of chemical bonds. These results confront positively the mode-coupling theory with a new control parameter.

RESUMEN

The high-frequency acoustic dynamics of sulfur across the liquid-liquid, lambda transition has been studied using inelastic x-ray scattering. The combination of these high-frequency data with lower frequency, literature data indicates that liquid sulfur develops, in the high-temperature, polymeric solution phase, some characteristic features of a rubber. In particular, entanglement coupling among polymeric chains plays a relevant role in the dynamics of this liquid phase.

RESUMEN

A dispersion-compensation method to remove the cube-size effect from the resolution function of diced analyzer crystals using a position-sensitive two-dimensional pixel detector is presented. For demonstration, a resolution of 23 meV was achieved with a spectrometer based on a 1 m Rowland circle and a diced Si(555) analyzer crystal in a near-backscattering geometry, with a Bragg angle of 88.5 degrees . In this geometry the spectrometer equipped with a traditional position-insensitive detector provides a resolution of 190 meV. The dispersion-compensation method thus allows a substantial increase in the resolving power without any loss of signal intensity.

Asunto(s)

RESUMEN

The dynamic structure factor of m-toluidine has been measured by inelastic x-ray scattering in the mesoscopic Q range between 1 and 10 nm(-1), where a prepeak is revealed in the static structure factor resulting from the existence of hydrogen bonded, nanometer size clusters. Evidence is given of (i) a square-root cusp in the nonergodicity factor and of (ii) critical nonergodicity parameters which oscillate in phase with the static structure factor. These results demonstrate that local order in a liquid can coexist with the signatures of the ergodic to nonergodic transition predicted by the mode coupling theory for simple, dense liquids.

RESUMEN

High-resolution, inelastic x-ray scattering measurements of the dynamic structure factor S (Q,omega) of liquid water have been performed for wave vectors Q between 4 and 30 nm(-1) in distinctly different thermodynamic conditions ( T=263-420 K ; at, or close to, ambient pressure and at P=2 kbar ). In agreement with previous inelastic x-ray and neutron studies, the presence of two inelastic contributions (one dispersing with Q and the other almost nondispersive) is confirmed. The study of their temperature and Q dependence provides strong support for a dynamics of liquid water controlled by the structural relaxation process. A viscoelastic analysis of the Q -dispersing mode, associated with the longitudinal dynamics, reveals that the sound velocity undergoes a complete transition from the adiabatic sound velocity ( c(0) ) (viscous limit) to the infinite-frequency sound velocity ( c(infinity) ) (elastic limit). On decreasing Q , as the transition regime is approached from the elastic side, we observe a decrease of the intensity of the second, weakly dispersing feature, which completely disappears when the viscous regime is reached. These findings unambiguously identify the second excitation to be a signature of the transverse dynamics with a longitudinal symmetry component, which becomes visible in S (Q,omega) as soon as the purely viscous regime is left.

RESUMEN

We discuss the microscopic dynamics and structure of liquid hydrogen and deuterium, as probed by inelastic x-ray scattering measurements. Samples are kept in corresponding thermodynamic conditions, at which classical systems are expected to exhibit the same dynamic and static responses. On the contrary, we observe clear differences revealing the onset of quantum deviations, both in the broadening of inelastic excitations and in the position of the first sharp diffraction peak. These features are discussed, compared to path-integral Monte Carlo simulations, and finally associated with the different de Broglie wavelengths of the two isotopes.

RESUMEN

We report on inelastic x-ray scattering experiments on crystalline and glassy phases of ethanol in order to directly compare the influence of disorder on high frequency acoustic excitations. We find that both the dispersion and the line-width of the longitudinal acoustic excitations in the glass are the same as in the polycrystal in the reciprocal space portion covering the 1st and 2nd Brillouin zones. The structural disorder is found to play little role apart from an intrinsic angular averaging, and the nature of these excitations must essentially be the same in both glass and poly crystal.

RESUMEN

The high-frequency sound velocity v( infinity ) of liquid water has been determined to densities of 1.37 g/cm(3) by inelastic x-ray scattering. In comparison to the hydrodynamic sound velocity v(0), the increase of v( infinity ) with density is substantially less pronounced, indicating that, at high density, the hydrogen-bond network is decreasingly relevant to the physical properties of liquid water. Furthermore, we observe an anomaly in v( infinity ) at densities around 1.12 g/cm(3), contrasting the smooth density evolution of v(0).

RESUMEN

The high frequency collective dynamics of liquid hydrogen fluoride is studied by inelastic x-ray scattering on the coexistence curve at T = 239 K. The comparison with existing molecular dynamics simulations shows the existence of two active relaxation processes with characteristic time scales in the subpicosecond range. The observed scenario is very similar to that found in liquid water. This suggests that hydrogen bonded liquids behave similarly to other very different systems as simple and glass forming liquids, thus indicating that these two relaxation processes are universal features of the liquid state.

RESUMEN

An inelastic x-ray scattering (IXS) experiment in liquid neon has been performed in the +/-100 meV exchanged energy range and at exchanged wave numbers, q, comprised between 1 and 16 A(-1). At the highest probed q's a deep inelastic scattering regime is reached where the Ne core electrons, after collision with the x rays, recoil almost freely with an effective mass equal to the Ne atomic mass. IXS in this high q regime is here shown to provide quantitative information on the atomic momentum distribution of liquid Ne, thus supplying a complementary technique to neutron scattering. There are several open problems in quantum and classical liquids which can benefit from this complementarity.

RESUMEN

Quantum effects in the teraherz dynamics of supercritical 4He have been studied as a function of both density rho and temperature T; they have been characterized through their effects on the second and third spectral moments of the dynamic structure factor S(Q, omega), measured by the inelastic x-ray scattering (IXS) technique. The IXS spectra were collected in the low-Q region below and around the position of the first diffraction peak Q(m), i.e., in a range relatively unusual in this kind of investigation. The measured spectral moments clearly show a departure from their high-T classical expected values. We observe, moreover, that the amplitude of quantum deviations increases slightly with increasing density. This experimental method allows us to extract, even in a region where the dynamics still maintains a collective character, such typical single particle properties as the mean atomic kinetic energy.

RESUMEN

The dynamics structure factor S(Q,E) of liquid ammonia l-NH3 at T = 200 K and at its vapor pressure has been measured by inelastic x-ray scattering (IXS) in the 1-15 nm(-1) momentum transfer ( Q) range. Contrary to previous IXS studies on other associated liquids and glasses, in l-NH3 a large inelastic signal is observed up to Q = 15 nm(-1). This, enabling S(Q,E) measurements as a function of Q at constant E transfer, allows us to demonstrate experimentally the transition from a propagating dynamics regime, where the acoustic excitation energy linearly disperses with Q, to a high-Q regime, where it is no longer possible to observe a dominant excitation in the S(Q,E).