What is moving in silica at 1 K? A computer study of the low-temperature anomalies

Though the existence of two-level systems (TLS) is widely accepted to explain low temperature anomalies in many physical observables, knowledge about their properties is very rare. For silica which is one of the prototype glass-forming systems we elucidate the properties of the TLS via computer simulations by applying a systematic search algorithm. We get specific information in the configuration space, i.e. about relevant energy scales, the absolute number of TLS and electric dipole moments. Furthermore important insight about the real-space realization of the TLS can be obtained. Comparison with experimental observations is included

Loss of control in pattern-directed nucleation: a theoretical study

The properties of template-directed nucleation are studied close to the transition where full nucleation control is lost and additional nucleation occurs beyond the pre-patterned regions. First, kinetic Monte Carlo simulations are performed to obtain information on a microscopic level. Here the experimentally relevant cases of 1D stripe patterns and 2D square lattice symmetry are considered. The nucleation properties in the transition region depend in a complex way on the parameters of the system, i.e. the flux, the surface diffusion constant, the geometric properties of the pattern and the desorption rate. Second, the properties of the stationary concentration field in the fully controlled case are studied to derive the remaining nucleation probability and thus to characterize the loss of nucleation control. Using the analytically accessible solution of a model system with purely radial symmetry, some of the observed properties can be rationalized. A detailed comparison to the Monte Carlo data is included

Diffusion of oxygen in Mg-doped α-Al2O3: the corundum conundrum explained

It has been a puzzle for over two decades that the enhancement of oxygen diffusion in α-Al_{2}O_{3} ,with respect to the amount of Mg doping, is several orders of magnitude less than expected. The standard model, which envisages that transport is mediated by oxygen vacancies induced to compensate the charge of Mg 2+ ions substituting Al 3+ ions, has not been able to explain this anomaly. Here, we report a detailed study of populations of point defects and defect clusters in Mg-doped α-Al_{2}O_{3}. By taking into account calculated defect formation energies from the literature, the condition of charge neutrality, and the environmental parameters (chemical potentials) under which the anomalous trend in oxygen diffusivities were previously observed, we are able to arrive at an explanation. A non-linear relationship between Mg concentration in the system and key native point defects, which serve as mediators of self-diffusion in α-Al_{2}O_{3_ , is predicted: the concentrations of such defects increase much more slowly in the supersaturation regime than in the pre-saturation regime, matching the anomalous result previously observed in α-Al_{2}O_{3} . We identify the reason for this as buffering by positively charged Mg interstitials and Mg–oxygen vacancy clusters, which compensate the negative charges of Mg substitutional defects (Mg^{1−}Al ). This study answers part of the long-standing question about self-diffusion in alumina, referred to by Heuer and Lagerlöf in 1999 as the Corundum Conundrum

Backward correlations and dynamic heterogeneities: a computer study of ion dynamics

We analyse the correlated back and forth dynamics and dynamic heterogeneities, i.e. the presence of fast and slow ions, for a lithium metasilicate system via computer simulations. For this purpose we define, in analogy to previous work in the field of glass transition, appropriate three-time correlation functions. They contain information about the dynamics during two successive time intervals. First we apply them to simple model systems in order to clarify their information content. Afterwards we use this formalism to analyse the lithium trajectories. A strong back-dragging effect is observed, which also fulfills the time-temperature superposition principle. Furthermore, it turns out that the back-dragging effect is long-ranged and exceeds the nearest neighbor position. In contrast, the strength of the dynamic heterogeneities does not fulfill the time-temperature superposition principle. The lower the temperature, the stronger the mobility difference between fast and slow ions. The results are then compared with the simple model systems considered here as well as with some lattice models of ion dynamics.Comment: 12 pages, 10 figure

Characterization of local dynamics and mobilities in polymer melts - a simulation study

The local dynamical features of a PEO melt studied by MD simulations are compared to two model chain systems, namely the well-known Rouse model as well as the semiflexible chain model (SFCM) that additionally incorporates chain stiffness. Apart from the analysis of rather general quantities such as the mean square displacement (MSD), we present a new statistical method to extract the local bead mobility from the simulation data on the basis of the Langevin equation, thus providing a complementary approach to the classical Rouse-mode analysis. This allows us to check the validity of the Langevin equation and, as a consequence, the Rouse model. Moreover, the new method has a broad range of applications for the analysis of the dynamics of more complex polymeric systems like comb-branched polymers or polymer blends.Comment: 6 pages, 5 figure

Finite-Size Effects in a Supercooled Liquid

We study the influence of the system size on various static and dynamic properties of a supercooled binary Lennard-Jones liquid via computer simulations. In this way, we demonstrate that the treatment of systems as small as N=65 particles yields relevant results for the understanding of bulk properties. Especially, we find that a system of N=130 particles behaves basically as two non-interacting systems of half the size.Comment: Proceedings of the III Workshop on Non Equilibrium Phenomena in Supercooled Fluids, Glasses and Amorphous Materials, Sep 2002, Pis

Specific heat of two-dimensional diluted magnets

Using Monte Carlo techniques, the two-dimensional site-diluted Ising model is studied. In particular, properties of the specific heat, its critical behaviour and the emergence of a non-singular maximum above the transition temperature at moderate concentration of defects, are discussed.Comment: 10 pages, 5 eps-figures, elsart-style, submitted to Physica