High frequency dynamics in liquids and supercritical fluids: A comparative inelastic x-ray scattering study.

The microscopic dynamics of four prototype systems (water, ammonia, nitrogen, and neon) across the critical temperature has been investigated by means of high-resolution inelastic x-ray scattering. The experimental line shape has been described using a model based on the memory function formalism. Two main relaxations, the thermal and the structural one, were observed in all the investigated systems. We found that the microscopic mechanism driving the structural relaxation clearly changes, being mainly governed by intermolecular bond rearrangements below the critical temperature and by binary collisions above it. Moreover, we observed that the relative weight of the thermal relaxation systematically increases on approaching the critical temperature, thus allowing for the observation of a transition from an adiabatic to an isothermal regime of sound propagation. Finally, we found the presence of an additional instantaneous relaxation, likely related to the coupling between collective vibrational modes and intramolecular degrees of freedom.

Nonlinear optics in the X-ray regime: nonlinear waves and self-action effects.

We study the nonlinear refraction of X-rays in highly ionized condensed matter by using a classical model of a cold electron plasma in a lattice of still ions coupled with Maxwell equations. We discuss the existence and stability of nonlinear waves. As a real-world example, we consider beam self-defocusing in crystalline materials (B, C, Li, Na). We predict that nonlinear processes become comparable to the linear ones for focused beams with powers of the order of mc(3)/ro (approximately 10 GW), the classical electron power. As a consequence, nonlinear phenomena are expected in currently exploited X-ray Free-Electron Lasers and in their future developments.

High-frequency dynamics of liquid and supercritical water.

The dynamic structure factor S(Q,omega) of water has been determined by high-resolution inelastic x-ray scattering (IXS) in a momentum (Q) and energy (E) transfer range extending from 2 to 4 nm{-1} and from +/-40meV . IXS spectra have been recorded along an isobaric path (400bar) in a temperature (T) interval ranging from ambient up to supercritical (T>647K) conditions. The experimental data have been described in the frame of the generalized hydrodynamic theory, utilizing a model based on the memory function approach. This model allows identifying the active relaxation processes which affect the time decay of density fluctuations, as well as a direct determination of the Q , T , and density (rho) dependencies of the involved transport parameters. The experimental spectra are well described by considering three different relaxation processes: the thermal, the structural, and the instantaneous one. On approaching supercritical conditions, we observe that the microscopic mechanism responsible for the structural relaxation is no longer related to the making and breaking of intermolecular bonds, but to binary intermolecular collisions.

High-frequency longitudinal and transverse dynamics in water.

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.

Experimental evidence of the acousticlike character of the high frequency excitations in glasses

The dynamic structure factor S(Q,E) of glassy glycerol has been measured by inelastic x-ray scattering as a function of momentum transfer Q and at constant energy transfer E. This allows one to establish independently from specific models of S(Q,E) the following: (i) Propagating collective excitations exist in glasses at high Q. (ii) Their dispersion up to E higher than E(BP) (the boson peak energy) confirms that E(BP) is not the onset of modes localization. (iii) The observation of an almost Q independent plateau on the high Q side of the Brillouin peak supports numerical simulations on glasses, describing the vibrational eigenvectors in terms of acousticlike and "random" components.

Determination of the short-wavelength propagation threshold in the collective excitations of liquid ammonia

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).

Nature of the short wavelength excitations in vitreous silica: An X-Ray brillouin scattering study

The dynamical structure factor [ S(Q,E)] of vitreous silica has been measured by inelastic x-ray scattering varying the exchanged wave vector ( Q) at fixed exchanged energy ( E)-an experimental procedure that, contrary to the usual one at constant Q, provides spectra with much better identified inelastic features. This allows us to obtain the first direct evidence of Brillouin peaks in the S(Q,E) of SiO2 at energies above the boson peak (BP) energy, a finding that excludes the possibility that the BP marks the transition from propagating to localized dynamics in glasses.

Evidence of short-time dynamical correlations in simple liquids.

We report a molecular dynamics study of the collective dynamics of a simple monatomic liquid--interacting through a two-body potential that mimics that of lithium--across the liquid-glass transition. In the glassy phase we find evidences of a fast relaxation process similar to that recently found in Lennard-Jones glasses. The origin of this process is ascribed to the topological disorder, i.e., to the dephasing of the different momentum Q Fourier components of the actual normal modes of vibration of the disordered structure. More important, we find that the fast relaxation persists in the liquid phase with almost no temperature dependence of its characteristic parameters (strength and relaxation time). We conclude, therefore, that in the liquid phase well above the melting point, at variance with the usual assumption of uncorrelated binary collisions, the short time particle motion is strongly correlated and can be described via a normal mode expansion of the atomic dynamics.

Inelastic x-ray scattering study of the collective dynamics in liquid sodium.

Inelastic x-ray scattering data have been collected for liquid sodium at T=390 K, i.e., slightly above the melting point. Owing to the very high instrumental resolution, pushed up to 1.5 meV, it has been possible to determine accurately the dynamic structure factor S(Q,omega) in a wide wave-vector range, 1.5-15 nm(-1), and to investigate on the dynamical processes underlying the collective dynamics. A detailed analysis of the line shape of S(Q,omega), similarly to other liquid metals, reveals the coexistence of two different relaxation processes with slow and fast characteristic time scales. The present data lead to the conclusion that (i) the picture of the relaxation mechanism based on a simple viscoelastic model fails and (ii) although the comparison with other liquid metals reveals similar behavior, the data do not exhibit an exact scaling law as the principle of the corresponding state would predict.

Quantum effects in the dynamics of He probed by inelastic x-ray scattering.

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.

Activity of epomediol in the treatment of hepatopathies: a double-blind multi-centre study.

A multi-centre study with epomediol discoids (200 mg three times daily for 30 days) versus placebo was carried out in 519 patients either with symptoms attributable to hepatopathy and/or alterations in the hepatic function. Epomediol was given to 257 patients chosen at random and the remaining 262 were given placebo. In cases of hepatopathy in which there was no severe damage to the hepatic parenchyma the symptoms of the disease were reduced and the laboratory parameters were improved on treatment with epomediol, whereas the activity of the drug was low in patients with chronic hepatopathy. This confirms that the clinical use of epomediol is most useful in cases of hepatopathy in which the change in hepatic function is still reversible.

[The otilonium bromide-benzodiazepine combination in the therapy of the irritable colon syndrome]. / L'associazione ottilionio bromuro-benzodiazepina nella terapia della sindrome del colon irritabile.

The irritable bowel syndrome is classified ad "disturbance of intestinal motility without an identifiable anatomic substrate". However, the clear etiopathogenetic implications of a psychosomatic nature complicate the search for an adequate therapeutic strategy. Based on this clinical experience, we set out to check the importance of a spasmolytic with a benzodiazepine and the tolerability of this type of combination. We therefore compared the results in 60 patients with irritable bowel syndrome of 8 weeks' treatment with tablets containing octylonium bromide (OB) 20 mg plus diazepam (DZ) 2 mg or OB 40 mg + 2 mg DZ. The doubling of the spasmolytic without increasing the daily dose of anxiolytic appeared to be useful for reducing the symptoms typical for the irritable bowel syndrome. In addition, the combination was found to be perfectly tolerated.