Water exists in high- and low-density amorphous ice forms (HDA and LDA), which could correspond to the glassy states of high- (HDL) and low-density liquid (LDL) in the metastable part of the phase diagram. However, the nature of both the glass transition and the high-to-low-density transition are debated and new experimental evidence is needed. Here we combine wide-angle X-ray scattering (WAXS) with X-ray photon-correlation spectroscopy (XPCS) in the small-angle X-ray scattering (SAXS) geometry to probe both the structural and dynamical properties during the high-to-low-density transition in amorphous ice at 1 bar. By analyzing the structure factor and the radial distribution function, the coexistence of two structurally distinct domains is observed at = 125 K. XPCS probes the dynamics in momentum space, which in the SAXS geometry reflects structural relaxation on the nanometer length scale. The dynamics of HDA are characterized by a slow component with a large time constant, arising from viscoelastic relaxation and stress release from nanometer-sized heterogeneities. Above 110 K a faster, strongly temperature-dependent component appears, with momentum transfer dependence pointing toward nanoscale diffusion. This dynamical component slows down after transition into the low-density form at 130 K, but remains diffusive. The diffusive character of both the high- and low-density forms is discussed among different interpretations and the results are most consistent with the hypothesis of a liquid-liquid transition in the ultraviscous regime.

Recently it was shown that CO-filled ice is formed upon compression of CO-clathrate hydrate. Here we show two alternative routes of its formation, namely, by decompression of CO/ice VI mixtures at 250 K and by isobaric heating of CO/high-density amorphous ice mixtures at 0.5-1.0 GPa above 200 K. Furthermore, we show that filled ice may either transform into the clathrate at an elevated pressure or decompose to "empty" hexagonal ice at ambient pressure and low temperature. This complements the literature studies in which decomposition to ice VI was favoured at high pressures and low temperatures.

This work reports on frequency dependent ambient-pressure dielectric measurements of hyperquenched glassy water, ice IV, ice VI, as well as a CO2-filled clathrate hydrate, the latter featuring a chiral water network. The dipolar time scales and the spectral shapes of the loss spectra of these specimens are mapped out and compared with literature data on low-density and high-density amorphous ices as well as on amorphous solid water. There is a trend that the responses of the more highly dense amorphous ices are slightly more dynamically heterogeneous than those of the lower-density amorphous ices. Furthermore, practically all of the amorphous ices, for which broadband dielectric spectra are available, display a curved high-frequency wing. Conversely, the high-frequency flanks of the nominally pure ice crystals including ice V and ice XII can be characterized by an approximate power-law behavior. While the spectral shapes of the nominally pure ices thus yield some hints regarding their amorphicity or crystallinity, a comparison of their time scale appears less distinctive in this respect. In the accessible temperature range, the relaxation times of the crystalline ices are between those of low-density and high-density amorphous ice. Hence, with reference also to previous work, the application of suitable doping currently seems to be the best dielectric spectroscopy approach to distinguish amorphous from crystalline ices.

Cracks and decomposition barriers observed in time-lapse micro-computed tomography measurements challenge existing models of gas hydrate decomposition.

Recently a new gas hydrate structure has been discovered. This structure, sX, is unique in a sense that it is so far the only gas hydrate with chiral channels. It is formed by hydrogen-water or carbon dioxide-water mixtures at pressures above 0.300 GPa and it has been shown that it is the only clathrate hydrate that is refillable with hydrogen. This property makes it a possible storage material for gases. By analysing neutron diffraction data and calculations based on density-functional theory, we show that sX is also refillable with nitrogen; the guest:host ratio will be shown to be 2.6(3). Furthermore, we report sX's decomposition behaviour and give evidence that it undergoes several transitions into the exotic hydrates sH and sIII that have not been observed at these pressure and temperature conditions-before forming the stable nitrogen hydrate sII.

Quantitative single crystal neutron-diffraction in diamond anvil cells has so far been to limited by the neutron flux available at the various neutron sources. As a result, highly precise measurements of the exact position of light elements have not been possible preventing, for example, structural studies of hydrogen and hydrogen bonds under pressure. Here we report experiments carried out on SNAP at the Spallation Neutron Source (ORNL, TN, USA) to explore the possibility and current limits of such studies. Furthermore, we benchmarked the obtained data quality with reference experiments carried out on TOPAZ, a dedicated single-crystal instrument. We show that measuring single-crystal diffraction intensities on SNAP is possible to such a precision that we are able to resolve the hydrogen bonds in potassium dideuterium phosphate (DKDP) as well as in ice VI.

<p>Our understanding on how opaque materials respond to extreme compression and high temperatures heavily relies on x-ray techniques. While X-ray diffraction is a powerful approach, some properties such as viscosity are experimentally not accessible with such approaches.  Application of x-ray imaging has been widely applied in extreme pressure and temperature conditions using multi-anvil presses, but obtaining sufficient space and time resolution for similar experiments using diamond anvil cells, at commensurately higher pressure and temperature conditions, have been challenging. We present recent developments in synchrotron X-ray imaging at the ECB beamline at PETRA III, DESY used in combination with laser heated DAC. Simultaneous X-ray imaging and diffraction allows for deeper insight in properties of materials under high pressure as well as the direct correspondence of phase transition diagnostics.  We present a case study of bismuth in the laser-heated diamond anvil cell showing detection of solid-solid and solid-liquid transitions and explore how X-ray imaging can be used to determine viscosity of molten bismuth under pressure.</p>

The mixed homonuclear and heteronuclear hydrogen bonds in ammonia hydrates have been of interest for several decades. In this manuscript, a neutron powder diffraction study is presented to investigate the structure of ammonia monohydrate IV at 170 K at an elevated pressure of 3–5 GPa. The most plausible structure that accounts for all features in the experimental pattern was found in the P21/c space group and has the lattice parameters a=5.487(3) Å, b=19.068(4) Å, c=5.989(3) Å, and β=99.537(16) deg. While the data quality limits discussion to a proton-ordered structure, the structure presented here sheds light on an important part of the ammonia–water phase diagram.