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Register a new userViscosity of Silica and Doped Silica Melts: Evidence for a Crossover Temperature
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Silica is known as the archetypal strong liquid, exhibiting an Arrhenius viscosity curve with a high glass transition temperature and constant activation energy. However, given the ideally isostatic nature of the silica network, the presence of even a small concentration of defects can lead to a significant decrease in both the glass transition temperature and activation energy for viscous flow. To understand the impact of trace level dopants on the viscosity of silica, we measure the viscosity-temperature curves for seven silica glass samples having different impurities, including four natural and three synthetic samples. Depending on the type of dopant, the glass transition temperature can vary by nearly 300 K. A common crossover is found for all viscosity curves around ~2200-2500 K, which we attribute to a change of the transport mechanism in the melt from being dominated by intrinsic defects at high temperature to dopant-induced defects at low temperatures.
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A previous inelastic UV scattering experiment on silica glass is reproduced using a high grade superpolished sample. In the pristine sample condition, surface scattering is not observable compared to Rayleigh scattering from the bulk. However, exposure to a fluence of the order of 100 J/cm$^2$ at photon energies slightly below the electronic gap generates observable surface damage. This occurs after a few hours illumination with the monochromatic spectrometer beam. No anomaly in the Brillouin linewidth was found up to an excitation energy of 7.8 eV.
We use textit{ab initio} molecular dynamics simulations to investigate the properties of the dry surface of pure silica and sodium silicate glasses. The surface layers are defined based on the atomic distributions along the direction ($z-$direction) perpendicular to the surfaces. We show that these surfaces have a higher concentration of dangling bonds as well as two-membered (2M) rings than the bulk samples. Increasing concentration of Na$_2$O reduces the proportion of structural defects. From the vibrational density of states, one concludes that 2M rings have a unique vibrational signature at a frequency $approx850$~cm$^{-1}$, compatible with experimental findings. We also find that, due to the presence of surfaces, the atomic vibration in the $z-$direction is softer than for the two other directions. The electronic density of states shows clear the differences between the surface and interior and we can attribute these to specific structural units. Finally, the analysis of the electron localization function allows to get insight on the influence of local structure and the presence of Na on the nature of chemical bonding in the glasses.
Silica, water and hydrogen are known to be the major components of celestial bodies, and have significant influence on the formation and evolution of giant planets, such as Uranus and Neptune. Thus, it is of fundamental importance to investigate their states and possible reactions under the planetary conditions. Here, using advanced crystal structure searches and first-principles calculations in the Si-O-H system, we find that a silica-water compound (SiO2)2(H2O) and a silica-hydrogen compound SiO2H2 can exist under high pressures above 450 and 650 GPa, respectively. Further simulations reveal that, at high pressure and high temperature conditions corresponding to the interiors of Uranus and Neptune, these compounds exhibit superionic behavior, in which protons diffuse freely like liquid while the silicon and oxygen framework is fixed as solid. Therefore, these superionic silica-water and silica-hydrogen compounds could be regarded as important components of the deep mantle or core of giants, which also provides an alternative origin for their anomalous magnetic fields. These unexpected physical and chemical properties of the most common natural materials at high pressure offer key clues to understand some abstruse issues including demixing and erosion of the core in giant planets, and shed light on building reliable models for solar giants and exoplanets.
We study shear stress relaxation for a gelling melt of randomly crosslinked, interacting monomers. We derive a lower bound for the static shear viscosity $eta$, which implies that it diverges algebraically with a critical exponent $kge 2 u-beta$. Here, $ u$ and $beta$ are the critical exponents of percolation theory for the correlation length and the gel fraction. In particular, the divergence is stronger than in the Rouse model, proving the relevance of excluded-volume interactions for the dynamic critical behaviour at the gel transition. Precisely at the critical point, our exact results imply a Mark-Houwink relation for the shear viscosity of isolated clusters of fixed size.
The recent synthesis and characterization of bilayers of vitreous silica has produced valuable new information on ring sizes and distributions. In this paper, we compare the ring statistics of experimental samples with computer generated samples. The average ring size is fixed at six by topology, but the width, skewness and other moments of the distribution of ring edges are characteristics of particular samples. We examine the Aboav-Weaire law that quantifies the propensity of smaller rings to be adjacent to larger rings, and find similar results for available experimental samples which however differ somewhat from computer-generated bilayers currently. We introduce a new law for the areas of rings of various sizes.
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