Onset of the alpha-relaxation in the glass-forming solution LiCl-6H2O revealed by Brillouin scattering techniques.

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.

Is there any fast sound in water?

We measured the dynamic structure factor S(Q,omega) of liquid and undercooled water down to 253 K in the Q approximately 0.02-0.1 nm;{-1} momentum transfer region. We observe the neat departure of the apparent speed of sound from the adiabatic regime as a function of decreasing temperature. Our evaluation of the infinite-frequency limit of sound velocity, c_{infinity}, matches with the results obtained in the high momentum transfer limit by inelastic neutron and x-ray scattering. These results strongly support the viscoelastic interpretation of the dynamics of water. Hence, we propose to call c_{infinity} the high-frequency speed of sound and to abandon the term fast sound, which recalls a propagation mechanism through lighter atoms, like in gas mixtures.

Evidence for a crossover in the frequency dependence of the acoustic attenuation in vitreous silica.

We report measurements of the sound attenuation coefficient in vitreous silica, for sound waves of wavelength between 50 and 80 nm, performed with the new inelastic UV light scattering technique. These data indicate that in silica glass a crossover between a temperature-dependent (at low frequency) and a temperature-independent (at high frequency) acoustic attenuation mechanism occurs at Q approximately equal to 0.15 nm(-1). The absence of any signature in the static structure factor at this Q value suggests that the observed crossover should be associated with local elastic constant fluctuations.

Crystal-like nature of acoustic excitations in glassy ethanol.

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.

Calorimetry at surfaces using high-resolution core-level photoemission.

We have developed a method to measure simultaneously the internal energy of bulk and the first layer atoms of a crystal. The internal energy of bulk and the surface atoms of lithium (110) have been evaluated from 22 K up to above the melting transition, applying the Debye model to the thermal broadening of the respective 1s photoemission lines. Our measurements clearly reveal two phase changes: the known liquid to solid transition and the surface melting, occurring 50 K below the bulk melting point.

Structural relaxation in liquid water by inelastic UV scattering.

Using the novel synchrotron radiation based inelastic ultraviolet scattering technique, the dynamic structure factor of normal and supercooled liquid water has been measured at a momentum transfer Q approximately equal to 0.1 nm(-1), in the temperature range 260-340 K. The structural (alpha) relaxation has been observed in the supercooled temperature region (T< or =273 K), where the inverse relaxation time matches the frequency of the probed sound modes. The T dependence of the relaxation time shows a diverging behavior with a critical temperature T approximately equal to 220 K. These results provide a unique experimental opportunity to frame the dynamics of water in the mode-coupling theory.

Inelastic ultraviolet scattering from high frequency acoustic modes in glasses.

The dynamic structure factor of vitreous silica and glycerol has been measured as a function of temperature and of the momentum transfer up to Q=0.105 nm(-1) using a novel experimental technique, the inelastic ultraviolet scattering. As in the case of Brillouin light scattering and ultrasonic measurements, the temperature dependence of the acoustic attenuation shows a plateau below the glass transition whose amplitude scales as Q2. Moreover, a slight temperature dependence of attenuation has been found in vitreous silica at about 130 K, which seems to be reminiscent of the peak measured at lower Qs. These two findings strongly support the idea that anharmonicity is responsible for sound attenuation at ultrasonic and hypersonic frequencies. Finally, we demonstrate that the attenuation mechanism should show a change of regime between 0.105 and 1 nm(-1).