A dense amorphous form of silica was prepared at high pressure from the highly compressible, siliceous zeolite, silicalite-1-F. Reverse Monte Carlo modeling of total X-ray scattering data shows that the structure of this novel amorphous form of SiO(2) recovered under ambient conditions is distinct from vitreous SiO(2) and retains the basic framework topology (i.e., chemical bonds) of the starting crystalline zeolite. This material is, however, amorphous over the different length scales probed by Raman and X-ray scattering due to strong geometrical distortions. This is thus an example of new topologically ordered, amorphous material with a different intermediate-range structure, a lower entropy with respect to a standard glass, and distinct physical and mechanical properties, eventually approaching those of an "ordered" or "perfect" glass. The same process in more complex aluminosilicate zeolites will, in addition, lead to an amorphous material which conserves the framework topology and chemical order of the crystal. The large volume collapse in this material may also be of considerable interest for new applications in shock wave absorption.

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International audienceIn situ X-ray diffraction and Raman spectroscopy measurements of synthetic powdered samples of faujasite 13X were carried out at high pressure using diamond anvil cells. Structural changes are detected, linked to a progressive reduction in crystallinity, before complete amorphization of the material. Three distinct compressibility regions are clearly observed, delimited by two discontinuities in the pressure dependence of the faujasite volume around 2 and 3.5 GPa. The transition from the crystal to the amorphous state is incomplete and partially reversible below pressures of between 8 and 12 GPa, depending on the pressure-transmitting medium used. This partial recovery of the initial structure, at least on a local level, could be related to the presence of hydrated sodium ions in the faujasite framework. In addition, the position of the first sharp diffraction peak in the X-ray diffraction pattern of a fully amorphous sample recovered from 24 GPa is consistent with the presence of 4-membered rings of tetrahedra and the persistence of a significant number of larger rings as compared to a dried amorphous faujasite precursor

Physical properties of solid methane have been studied at room temperature under high pressure in a diamond-anvil cell. Internal modes have been followed up to 20 GPa by Raman scattering. The refractive index has been measured by a newly developed method up to 12 GPa and the elastic properties determined by Brillouin scattering up to 32 GPa. In the plastic phase I, the experimental equation of state and the elastic properties were analyzed with reference to rare-gas solids, i.e. , with use of self-consistent harmonic calculations with various pair potentials. The best agreement is obtained with Aziz s Hartree-Fock+dispersion -C krypton-krypton potential. From analogies with rare-gas and NH3 solids, a hcp structure is proposed for phase IV. The IV-VII phase transition is shown to be orientational in nature.

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Confined H2O molecules act as local probes for depressurization phenomena during the pressure induced amorphisation of faujasite NaX at which the OH stretching frequency first decreases and then increases almost to its room pressure value upon further compression. Pair distribution function (PDF) analysis provides evidence that amorphisation corresponds to a collapse of the structure around hydrated sodium cations with strong distortion of the secondary building units (double six-membered rings, sodalite cages). Both the use of guest molecules as local probes in far- and mid-infrared spectroscopy, where we correlate intermolecular water H bonding vibrations and internal mode behaviour under confinement, and PDF analysis could be of great use to study the mechanical behaviour of other hydrated materials.

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