0000000000315651
AUTHOR
Andreas Heuer
Dynamical heterogeneities in glass-forming materials
ABSTRACTCooperative dynamics around the glass transition leads to complex motional behavior of the individual molecules, resulting in non-exponential relaxation. The nature of this non-exponentiality is clarified theoretically as well as experimentally. The non-exponentiality may be due to heterogeneous relaxation (superposition of exponential processes with different rate constants) or homogeneous relaxation (identical intrinsically non-exponential processes). A precise definition of both limits is given. It is shown that the type of relaxation, i.e. to which degree heterogeneous and homogeneous contributions are present, reflects geometrical properties of the dynamics. The heterogeneous c…
Memory effects in the relaxation of the Gaussian trap model
We investigate the memory effect in a simple model for glassy relaxation, a trap model with a Gaussian density of states. In this model thermal equilibrium is reached at all finite temperatures and therefore we can consider jumps from low to high temperatures in addition to the quenches usually considered in aging studies. We show that the evolution of the energy following the Kovacs-protocol can approximately be expressed as a difference of two monotonously decaying functions and thus show the existence of a so-called Kovacs hump whenever these functions are not single exponentials. It is well established that the Kovacs effect also occurs in the linear response regime and we show that mos…
Aging effects manifested in the potential-energy landscape of a model glass former
We present molecular dynamics simulations of a model glass-forming liquid (the binary Kob-Anderson Lennard-Jones model) and consider the distributions of inherent energies and metabasins during aging. In addition to the typical protocol of performing a temperature jump from a high temperature to a low destination temperature, we consider the temporal evolution of the distributions after an 'up-jump', i.e. from a low to a high temperature. In this case the distribution of megabasin energies exhibits a transient two-peak structure. Our results can qualitatively be rationalized in terms of a trap model with a Gaussian distribution of trap energies. The analysis is performed for different syste…
Considerations on correlations in shift-register pseudorandom number generators and their removal
Abstract We present a simple calculation quantitatively explaining the triplet correlations in the popular shift-register random number generator “R250”, which were recently observed numerically by Schmid and Wilding, and are known from general analysis of this type of generator. Starting from these considerations, we discuss various methods to remove these correlations by combining different shift-register generators. We implement and test a particularly simple and fast version, based on an XOR combination of two independent shift-register generators with different time lags. The results indicate that this generator has much better statistical properties than R250, while being only a facto…
Nature of the non-exponential primary relaxation in structural glass-formers probed by dynamically selective experiments
Several experimental methods feature the potential to distinguish between slow and fast contributions to the non-exponential, ensemble averaged primary response in glass-forming materials. Some of these techniques are based on the selection of subensembles using multi-dimensional nuclear magnetic resonance, optical bleaching, and non-resonant spectral hole burning. Others, such as the time-dependent solvation spectroscopy, measure microscopic responses induced by local perturbations. Using several of these methods it could be demonstrated for various glass-forming materials that the non-exponential relaxation results from a superposition of dynamically distinguishable entities. The experime…