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Register a new userInduced glassy behavior in the melt of glycerol and aerosil dispersions
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Added by
Germano Iannacchione
Publication date
2005
fields
Physics
and research's language is
English
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A high-resolution calorimetric spectroscopy study has been performed on pure glycerol and colloidal dispersions of an aerosil in glycerol covering a wide range of temperatures from 300 K to 380 K, deep in the liquid phase of glycerol. The colloidal glycerol+aerosil samples with 0.05, 0.10, and 0.20 mass fraction of aerosil reveal glassy, activated dynamics at temperatures well above the $T_g$ of the pure glycerol. The onset of glass-like behavior appears to be due to the structural frustration imposed by the silica gel on the glycerol liquid. The aerosil gel increases the net viscosity of the mixture, placing the sample effectively at a lower temperature thus inducing a glassy state. Given the onset of this behavior at relatively low aerosil density (large mean-void length compared to the size of a glycerol molecule), this induced glassy behavior is likely due to a collective mode of glycerol molecules. The study of frustrated glass-forming systems may be a unique avenue for illuminating the physics of glasses.
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High-resolution ac-calorimetry has been carried out on dispersions of aerosils in the liquid crystal octyloxycyanobiphenyl (8OCB) as a function of aerosil concentration and temperature spanning the crystal to isotropic phases. The liquid-crystal 8OCB is elastically stiffer than the previously well studied octylcyanobiphenyl (8CB)+aerosil system and so, general quenched random disorder effects and liquid-crystal specific effects can be distinguished. A double heat capacity feature is observed at the isotropic to nematic phase transition with an aerosil independent overlap of the heat capacity wings far from the transition and having a non-monotonic variation of the transition temperature. A crossover between low and high aerosil density behavior is observed for 8OCB+aerosil. These features are generally consistent with those on the 8CB+aerosil system. Differences between these two systems in the magnitude of the transition temperature shifts, heat capacity suppression, and crossover aerosil density between the two regimes of behavior indicate a liquid crystal specific effect. The low aerosil density regime is apparently more orientationally disordered than the high aerosil density regime, which is more translationally disordered. An interpretation of these results based on a temperature dependent disorder strength is discussed. Finally, a detailed thermal hysteresis study has found that crystallization of a well homogenized sample perturbs and increases the disorder for low aerosil density samples but does not influence high density samples.
Liquid crystals offer many unique opportunities to study various phase transitions with continuous symmetry in the presence of quenched random disorder (QRD). The QRD arises from the presence of porous solids in the form of a random gel network. Experimental and theoretical work support the view that for fixed (static) inclusions, quasi-long-range smectic order is destroyed for arbitrarily small volume fractions of the solid. However, the presence of porous solids indicates that finite-size effects could play some role in limiting long-range order. In an earlier work, the nematic - smectic-A transition region of octylcyanobiphenyl (8CB) and silica aerosils was investigated calorimetrically. A detailed x-ray study of this system is presented in the preceding Paper I, which indicates that pseudo-critical scaling behavior is observed. In the present paper, the role of finite-size scaling and two-scale universality aspects of the 8CB+aerosil system are presented and the dependence of the QRD strength on the aerosil density is discussed.
We present a theoretical discussion of the reversible parking problem, which appears to be one of the simplest systems exhibiting glassy behavior. The existence of slow relaxation, nontrivial fluctuations, and an annealing effect can all be understood by recognizing that two different time scales are present in the problem. One of these scales corresponds to the fast filling of existing voids, the other is associated with collective processes that overcome partial ergodicity breaking. The results of the theory are in a good agreement with simulation data; they provide a simple qualitative picture for understanding recent granular compaction experiments and other glassy systems.
We propose a model Hamiltonian for describing charge transport through short homogeneous double stranded DNA molecules. We show that the hybridization of the overlapping pi orbitals in the base-pair stack coupled to the backbone is sufficient to predict the existence of a gap in the nonequilibrium current-voltage characteristics with a minimal number of parameters. Our results are in a good agreement with the recent finding of semiconducting behavior in short poly(G)-poly(C) DNA oligomers. In particular, our model provides a correct description of the molecular resonances which determine the quasi-linear part of the current out of the gap region.
Cooperative events requiring anomalously large fluctuations are a defining characteristic for the onset of glassy relaxation across many materials. The importance of such intermittent events has been noted in systems as diverse as superconductors, metallic glasses, gels, colloids, and granular piles. Here, we show that prohibiting the attainment of new record-high energy fluctuations -- by explicitly imposing a ``lid on the fluctuation spectrum -- impedes further relaxation in the glassy phase. This lid allows us to directly measure the impact of record events on the evolving system in extensive simulations of aging in such vastly distinct glass formers as spin glasses and tapped granular piles. Interpreting our results in terms of a dynamics of records succeeds in explaining the ubiquity of both, the logarithmic decay of the energy and the memory effects encoded in the scaling of two-time correlation functions of aging systems.
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