In this work the origin of permselectivity in dense silica films which possess a pore structure with pore sizes commensurate with the molecular size of the diffusing gas species is investigated. Much of the recently reported work in this field has involved the development of composite membrane films, and while it is generally assumed that the transport process of the gas species within the selective layer of these films is activated in nature, there are anomalies with this simplified picture. In this paper a new model is developed which, for the first time, explains the permselective behavior of the thin selective coatings ubiquitous to membrane separation processes. The model involves the existence of two primary transport domains within the solid film, one of which rapidly conducts the permeating gas (under non-Fickian conditions), while the second domain involves a slow diffusion mode characterized by normal Fickian transport. To validate the model, molecular dynamics simulations are conducted for diffusion of a number of simple gases (He, N(2), and CO(2)) within silica glasses over a range of solid densities. The silica media employed in these studies are based on a novel approach developed in this work for the construction of three-dimensionally periodic atomistic structures of silica of arbitrary density in which network bond connectivity is ensured. The results obtained from this work are in qualitative agreement with experimental observations and confirm the existence of dual mode transport which is central to the interpretation of the permselectivity in composite membranes systems.
Superconductivity is a result of quantum coherence at macroscopic scales. Two superconductors separated by a metallic or insulating weak link exhibit the AC Josephson effect -the conversion of a DC voltage bias into an AC supercurrent. This current may be used to activate mechanical oscillations in a suspended weak link. As the DC voltage bias condition is remarkably difficult to achieve in experiments, here we analyse theoretically how the Josephson effect can be exploited to activate and detect mechanical oscillations in the experimentally relevant condition with purely DC current bias. We unveil for the first time how changing the strength of the electromechanical coupling results in two qualitatively different regimes showing dramatic effects of the oscillations on the DC current-voltage characteristic of the device. These include the apperance of Shapirolike plateaux for weak coupling and a sudden mechanically-induced retrapping for strong coupling. Our predictions, measurable in state of the art experimental setups, allow the determination of the frequency and quality factor of the resonator using DC only techniques.
To distinguish thin deposited film characteristics clearly from the influence of substrate morphological properties, the growth mechanism and the macroscale and nanoscale properties of nanoporous SiO(2) films deposited on nonporous silica (SiO(2)) substrates from chemical precursors Si(OH)(4) and TEOS (tetraethoxysilane) via low-pressure chemical vapor deposition are the primary targets of this study. This work employs a kinetic Monte Carlo (KMC) simulation method coupled to the Metropolis Monte Carlo method to relax the strained silica structure. The influence of the deposition temperature (473, 673, and 873 K) on the properties of the SiO(x) layers is addressed via analysis of the film growth rates, density profiles of the deposited thin films, pore size distributions, carbon depth profiles (with respect to TEOS), and voidage analysis for layers of different thicknesses (8-18 nm). A comparison of simulation with experimental results is also carried out.
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