Matching Items (3)
Description
The structure of glass has been the subject of many studies, however some
details remained to be resolved. With the advancement of microscopic
imaging techniques and the successful synthesis of two-dimensional materials,
images of two-dimensional glasses (bilayers of silica) are now available,
confirming that this glass structure closely follows the continuous random
network model. These images provide complete in-plane structural information
such as ring correlations, and intermediate range order and with computer
refinement contain indirect information such as angular distributions, and
tilting.
This dissertation reports the first work that integrates the actual atomic
coordinates obtained from such images with structural refinement to enhance
the extracted information from the experimental data.
The correlations in the ring structure of silica bilayers are studied
and it is shown that short-range and intermediate-range order exist in such networks.
Special boundary conditions for finite experimental samples are designed so atoms
in the bulk sense they are part of an infinite network.
It is shown that bilayers consist of two identical layers separated by a
symmetry plane and the tilted tetrahedra, two examples of
added value through the structural refinement.
Finally, the low-temperature properties of glasses in two dimensions
are studied. This dissertation presents a new approach to find possible
two-level systems in silica bilayers employing the tools of rigidity theory
in isostatic systems.
details remained to be resolved. With the advancement of microscopic
imaging techniques and the successful synthesis of two-dimensional materials,
images of two-dimensional glasses (bilayers of silica) are now available,
confirming that this glass structure closely follows the continuous random
network model. These images provide complete in-plane structural information
such as ring correlations, and intermediate range order and with computer
refinement contain indirect information such as angular distributions, and
tilting.
This dissertation reports the first work that integrates the actual atomic
coordinates obtained from such images with structural refinement to enhance
the extracted information from the experimental data.
The correlations in the ring structure of silica bilayers are studied
and it is shown that short-range and intermediate-range order exist in such networks.
Special boundary conditions for finite experimental samples are designed so atoms
in the bulk sense they are part of an infinite network.
It is shown that bilayers consist of two identical layers separated by a
symmetry plane and the tilted tetrahedra, two examples of
added value through the structural refinement.
Finally, the low-temperature properties of glasses in two dimensions
are studied. This dissertation presents a new approach to find possible
two-level systems in silica bilayers employing the tools of rigidity theory
in isostatic systems.
ContributorsSadjadi, Seyed Mahdi (Author) / Thorpe, Michael F (Thesis advisor) / Beckstein, Oliver (Committee member) / Schmidt, Kevin E (Committee member) / Treacy, Michael Mj (Committee member) / Arizona State University (Publisher)
Created2018
Description
Amorphous phases are detected over large regions of the Martian surface from orbit and in more localized deposits by rovers on the surface. Amorphous silicates can be primary or secondary in origin, both having formed through very different processes, so the unambiguous identification of these phases is important for understanding the geologic history of Mars. Secondary amorphous silicates are poorly understood and underrepresented in spectral libraries because they lack the long-range structural order that makes their crystalline counterparts identifiable in most analytical techniques. Fortunately, even amorphous materials have some degree of short-range order so that distinctions can be made with careful characterization.
Two sets of laboratory experiments were used to produce and characterize amorphous weathering products under probable conditions for the Martian surface, and one global spectral analysis using thermal-infrared (TIR) data from the Thermal Emission Spectrometer (TES) instrument was used to constrain variations in amorphous silicates across the Martian surface. The first set of experiments altered crystalline and glassy basalt samples in an open system under strong (pH 1) and moderate (pH 3) acidic conditions. The second set of experiments simulated a current-day Martian weathering scenario involving transient liquid water where basalt glass weathering solutions, formed in circumneutral (pH ~5.5 and 7) conditions, were rapidly evaporated, precipitating amorphous silicates. The samples were characterized using visible and near-infrared (VNIR) spectroscopy, TIR spectroscopy, scanning electron microscopy (SEM), energy dispersive X-ray spectroscopy (EDS), and X-ray diffraction (XRD).
All experiments formed amorphous silicate phases that are new to spectral libraries. Moderately acidic alteration experiments produced no visible or spectral evidence of alteration products, whereas exposure of basalt glass to strongly acidic fluids produced silica-rich alteration layers that are spectrally consistent with VNIR and TIR spectra from the circum-polar region of Mars, indicating this region has undergone acidic weathering. Circum-netural pH basalt weathering solution precipitates are consistent with amorphous materials measured by rovers in soil and rock surface samples in Gale and Gusev Craters, suggesting transient water interactions over the last 3 billion years. Global spectral analyses determine that alteration conditions have varied across the Martian surface, and that alteration has been long lasting.
Two sets of laboratory experiments were used to produce and characterize amorphous weathering products under probable conditions for the Martian surface, and one global spectral analysis using thermal-infrared (TIR) data from the Thermal Emission Spectrometer (TES) instrument was used to constrain variations in amorphous silicates across the Martian surface. The first set of experiments altered crystalline and glassy basalt samples in an open system under strong (pH 1) and moderate (pH 3) acidic conditions. The second set of experiments simulated a current-day Martian weathering scenario involving transient liquid water where basalt glass weathering solutions, formed in circumneutral (pH ~5.5 and 7) conditions, were rapidly evaporated, precipitating amorphous silicates. The samples were characterized using visible and near-infrared (VNIR) spectroscopy, TIR spectroscopy, scanning electron microscopy (SEM), energy dispersive X-ray spectroscopy (EDS), and X-ray diffraction (XRD).
All experiments formed amorphous silicate phases that are new to spectral libraries. Moderately acidic alteration experiments produced no visible or spectral evidence of alteration products, whereas exposure of basalt glass to strongly acidic fluids produced silica-rich alteration layers that are spectrally consistent with VNIR and TIR spectra from the circum-polar region of Mars, indicating this region has undergone acidic weathering. Circum-netural pH basalt weathering solution precipitates are consistent with amorphous materials measured by rovers in soil and rock surface samples in Gale and Gusev Craters, suggesting transient water interactions over the last 3 billion years. Global spectral analyses determine that alteration conditions have varied across the Martian surface, and that alteration has been long lasting.
ContributorsSmith, Rebecca (Author) / Christensen, Philip R. (Philip Russel) (Thesis advisor) / Shock, Everett (Committee member) / Hartnett, Hilairy (Committee member) / Shim, Sang-Heon (Committee member) / Sharp, Thomas (Committee member) / Arizona State University (Publisher)
Created2016
Description
Zeolites are a class of microporous materials that are immensely useful as molecular sieves and catalysts. While there exist millions of hypothetical zeolite topologies, only 206 have been recognized to exist in nature, and the question remains: What distinguishes known zeolite topologies from their hypothetical counterparts? It has been found that all 206 of the known zeolites can be represented as networks of rigid perfect tetrahedra that hinge freely at the connected corners. The range of configurations over which the corresponding geometric constraints can be met has been termed the "flexibility window". Only a small percentage of hypothetical types exhibit a flexibility window, and it is thus proposed that this simple geometric property, the existence of a flexibility window, provides a reliable benchmark for distinguishing potentially realizable hypothetical structures from their infeasible counterparts. As a first approximation of the behavior of real zeolite materials, the flexibility window provides additional useful insights into structure and composition. In this thesis, various methods for locating and exploring the flexibility window are discussed. Also examined is the assumption that the tetrahedral corners are force-free. This is a reasonable approximation in silicates for Si-O-Si angles above ~135°. However, the approximation is poor for germanates, where Ge-O-Ge angles are constrained to the range ~120°-145°. Lastly, a class of interesting low-density hypothetical zeolites is evaluated based on the feasibility criteria introduced.
ContributorsDawson, Colby (Author) / Treacy, Michael M. J. (Thesis advisor) / O'Keeffe, Michael (Committee member) / Thorpe, Michael F. (Committee member) / Rez, Peter (Committee member) / Bennett, Peter (Committee member) / Arizona State University (Publisher)
Created2013