The frustration-based approach of supercooled liquids and the glass transition: a review and critical assessment

One of the most spectacular phenomena in physics in terms of dynamical range is the glass transition and the associated slowing down of flow and relaxation with decreasing temperature. That it occurs in many different liquids seems to call for a "universal" theory. In this article, we review one such theoretical approach which is based on the concept of "frustration". Frustration in this context describes an incompatibility between extension of the locally preferred order in a liquid and tiling of the whole space. We provide a critical assessment of what has been achieved within this approach and we discuss the relation with other theories of the glass transition.Comment: 48 pages, 13 figures, submitted to J. Phys : Cond. Matte

Recurrence networks - A novel paradigm for nonlinear time series analysis

This paper presents a new approach for analysing structural properties of time series from complex systems. Starting from the concept of recurrences in phase space, the recurrence matrix of a time series is interpreted as the adjacency matrix of an associated complex network which links different points in time if the evolution of the considered states is very similar. A critical comparison of these recurrence networks with similar existing techniques is presented, revealing strong conceptual benefits of the new approach which can be considered as a unifying framework for transforming time series into complex networks that also includes other methods as special cases. It is demonstrated that there are fundamental relationships between the topological properties of recurrence networks and the statistical properties of the phase space density of the underlying dynamical system. Hence, the network description yields new quantitative characteristics of the dynamical complexity of a time series, which substantially complement existing measures of recurrence quantification analysis

The role of local structure in dynamical arrest

Amorphous solids, or glasses, are distinguished from crystalline solids by their lack of long-range structural order. At the level of two-body structural correlations, glassformers show no qualitative change upon vitrifying from a supercooled liquid. Nonetheless the dynamical properties of a glass are so much slower that it appears to take on the properties of a solid. While many theories of the glass transition focus on dynamical quantities, a solid's resistance to flow is often viewed as a consequence of its structure. Here we address the viewpoint that this remains the case for a glass. Recent developments using higher-order measures show a clear emergence of structure upon dynamical arrest in a variety of glass formers and offer the tantalising hope of a structural mechanism for arrest. However a rigorous fundamental identification of such a causal link between structure and arrest remains elusive. We undertake a critical survey of this work in experiments, computer simulation and theory and discuss what might strengthen the link between structure and dynamical arrest. We move on to highlight the relationship between crystallisation and glass-forming ability made possible by this deeper understanding of the structure of the liquid state, and emphasize the potential to design materials with optimal glassforming and crystallisation ability, for applications such as phase-change memory. We then consider aspects of the phenomenology of glassy systems where structural measures have yet to make a large impact, such as polyamorphism (the existence of multiple liquid states), aging (the time-evolution of non-equilibrium materials below their glass transition) and the response of glassy materials to external fields such as shear.Comment: 70 page

Impacts of Mixed-Wettability on Brine Drainage and Supercritical CO2 Storage Efficiency in a 2.5-D Heterogeneous Micromodel

Geological carbon storage (GCS) involves unstable drainage processes, the formation of patterns in a morphologically unstable interface between two fluids in a porous medium during drainage. The unstable drainage processes affect CO2 storage efficiency and plume distribution and can be greatly complicated by the mixed-wet nature of rock surfaces common in hydrocarbon reservoirs where supercritical CO2 (scCO2) is used in enhanced oil recovery. We performed scCO2 injection (brine drainage) experiments at 8.5 MPa and 45°C in heterogeneous micromodels, two mixed-wet with varying water- and intermediate-wet patches, and one water-wet. The flow regime changes from capillary fingering through crossover to viscous fingering in the micromodels of the same pore geometry but different wetting surfaces at displacement rates with logCa (capillary number) increasing from −8.1 to −4.4. While the mixed-wet micromodel with uniformly distributed intermediate-wet patches yields ~0.15 scCO2 saturation increase at both capillary fingering and crossover flow regimes (−8.1 ≤ logCa ≤ − 6.1), the one heterogeneous wetting to scCO2 results in ~0.09 saturation increase only at the crossover flow regime (−7.1 ≤ logCa ≤ − 6.1). The interconnected flow paths in the former are quantified and compared to the channelized scCO2 flow through intermediate-wet patches in the latter by topological analysis. At logCa > − 6.1 (near well), the effects of wettability and pore geometry are suppressed by strong viscous force. Both scCO2 saturation and distribution suggest the importance of wettability on CO2 storage efficiency and plume shape in reservoirs and capillary leakage through caprock at GCS conditions

Critical point network for drainage between rough surfaces

In this paper, we present a network method for computing two-phase flows between two rough surfaces with significant contact areas. Low-capillary number drainage is investigated here since one-phase flows have been previously investigated in other contributions. An invasion percolation algorithm is presented for modeling slow displacement of a wetting fluid by a non wetting one between two rough surfaces. Short-correlated Gaussian process is used to model random rough surfaces.The algorithm is based on a network description of the fracture aperture field. The network is constructed from the identification of critical points (saddles and maxima) of the aperture field. The invasion potential is determined from examining drainage process in a flat mini-channel. A direct comparison between numerical prediction and experimental visualizations on an identical geometry has been performed for one realization of an artificial fracture with a moderate fractional contact area of about 0.3. A good agreement is found between predictions and observations

Viscosity and glass transition in amorphous oxides

An overview is given of amorphous oxide materials viscosity and glass-liquid transition phenomena. The viscosity is a continuous function of temperature, whereas the glass-liquid transition is accompanied by explicit discontinuities in the derivative parameters such as the specific heat or thermal expansion coefficient. A compendium of viscosity models is given including recent data on viscous flow model based on network defects in which thermodynamic parameters of configurons—elementary excitations resulting from broken bonds—are found from viscosity-temperature relationships. Glass-liquid transition phenomena are described including the configuron model of glass transition which shows a reduction of Hausdorff dimension of bonds at glass-liquid transition