Reply to the Comment of Muessel and Rieger on ``Aging Effects in a Lennard-Jones Glass''

This is a Reply to the Comment of Muessel and Rieger cond-mat/9804063 to out paper on ``Aging Effects in a Lennerd-Jones Glass''. We show that the scaling function proposed by Muessel and Rieger does not lead to a satisfactory scaling of our aging data.Comment: 1 page of Revtex, 1 eps figur

Non-linear dynamic response of glass-forming liquids to random pinning

We use large scale computer simulations of a glass-forming liquid in which a fraction c of the particles has been permanently pinned. We find that the relaxation dynamics shows an exponential dependence on c. This result can be rationalized by means of a simple theoretical Ansatz and we discuss its implication for thermodynamic theories for the glass-transition. For intermediate and low temperatures we find that the slowing down of the dynamics due to the pinning saturates and that the cooperativity decreases with increasing c, results which indicate that in glass-forming liquids there is a dynamic crossover at which the shape of the relaxing entities changes

The relaxation dynamics of a viscous silica melt: II The intermediate scattering functions

We use molecular dynamics computer simulations to study the relaxation dynamics of a viscous melt of silica. The coherent and incoherent intermediate scattering functions, F_d(q,t) and F_s(q,t), show a crossover from a nearly exponential decay at high temperatures to a two-step relaxation at low temperatures. Close to the critical temperature of mode-coupling theory (MCT) the correlators obey in the alpha-regime the time temperature superposition principle (TTSP) and show a weak stretching. We determine the wave-vector dependence of the stretching parameter and find that for F_d(q,t) it shows oscillations which are in phase with the static structure factor. The temperature dependence of the alpha- relaxation times tau shows a crossover from an Arrhenius law at low temperatures to a weaker T-dependence at intermediate and high temperatures. At the latter temperatures the T-dependence is described well by a power law. We find that the exponent gamma of the power law for tau are significantly larger than the one for the diffusion constant. The q-dependence of the alpha-relaxation times for F_d(q,t) oscillates around tau(q) for F_s(q,t) and is in phase with the structure factor. Due to the strong vibrational component of the dynamics at short times the TTSP is not valid in the beta- relaxation regime. We show, however, that in this time window the shape of the curves is independent of the correlator and is given by a functional form proposed by MCT. We find that the value of the von Schweidler exponent and the value of gamma for finite q are compatible with the expression proposed by MCT. We conclude that, in the temperature regime where the relaxation times are mesoscopic, many aspects of the dynamics of this strong glass former can be rationalized very well by MCT.Comment: 31 pages of Latex, 14 figure

Replica-exchange molecular dynamics simulation for supercooled liquids

We investigate to what extend the replica-exchange Monte Carlo method is able to equilibrate a simple liquid in its supercooled state. We find that this method does indeed allow to generate accurately the canonical distribution function even at low temperatures and that its efficiency is about 10-100 times higher than the usual canonical molecular dynamics simulation.Comment: 6 pages, 5 figure

Structuring polymer gels via catalytic reactions

We use computer simulations to investigate how a catalytic reaction in a polymer sol can induce the formation of a polymer gel. To this aim we consider a solution of homopolymers in which freely-diffusing catalysts convert the originally repulsive A monomers into attractive B ones. We find that at low temperatures this reaction transforms the polymer solution into a physical gel that has a remarkably regular mesostructure in the form of a cluster phase, absent in the usual homopolymer gels obtained by a quench in temperature. We investigate how this microstructuring depends on catalyst concentration, temperature, and polymer density and show that the dynamics for its formation can be understood in a semi-quantitative manner using the interaction potentials between the particles as input. The structuring of the copolymers and the AB sequences resulting from the reactions can be discussed in the context of the phase behaviour of correlated random copolymers. The location of the spinodal line as found in our simulations is consistent with analytical predictions. Finally, we show that the observed structuring depends not only on the chemical distribution of the A and B monomers but also on the mode of formation of this distribution