arXiv subjects

Jeppe C. Dyre

Publications and source records attributed to Jeppe C. Dyre.

At least 163 records · Page 9Linked to original sources

arXiv2006

Violations of conservation laws in viscous liquid dynamics

The laws expressing conservation of momentum and energy apply to any isolated system, but these laws are violated for for highly viscous liquids under laboratory conditions because of the unavoidable interactions with the measuring equipment over the long times needed to study the dynamics. Although particle number conservation applies strictly for any liquid, the solidity of viscous liquids implies that even this conservation law is apparently violated in coarse-grained descriptions of density fluctuations.

cond-mat.soft↗

arXiv2006

An energy landscape model for glass forming liquids in three dimensions

We present a three-dimensional lattice-gas model with trivial thermodynamics, but nontrivial dynamics. The model is characterized by each particle having its own random energy landscape. The equilibrium dynamics of the model were investigated by continuous time Monte Carlo simulations at two different densities at several temperatures. At high densities and low temperatures the model captures the important characteristics of viscous liquid dynamics. We thus observe non-exponential relaxation in the self part of the density auto-correlation function, and fragility plots of the self-diffusion constant and relaxation times show non-Arrhenius behavior.

cond-mat.soft↗

arXiv2006

Elastic models for the non-Arrhenius viscosity of glass-forming liquids

This paper first reviews the shoving model for the non-Arrhenius viscosity of viscous liquids. According to this model the main contribution to the activation energy of a flow event is the energy needed for molecules to shove aside the surrounding, an energy which is proportional to the instantaneous shear modulus of the liquid. Data are presented supporting the model. It is shown that the fractional Debye-Stokes-Einstein relation, that quantitatively expresses the frequently observed decoupling of, e.g., conductivity from viscous flow, may be understood within the model. The paper goes on to review several related explanations for the non-Arrhenius viscosity. Most of these are also "elastic models," i.e., they express the viscosity activation energy in terms of short-time elastic properties of the liquid. Finally, two new arguments for elastic models are given, a general solid-state defect argument and an Occam's razor type argument.

cond-mat.soft↗

arXiv2006

Elastic Models for the Non-Arrhenius Relaxation Time of Glass-Forming Liquids

We first review the phenomenology of viscous liquids and the standard models used for explaining the non-Arrhenius average relaxation time. Then the focus is turned to the so-called elastic models, arguing that these models are all equivalent in the Einstein approximation (where the short-time elastic properties are all determined by just one effective, temperature-dependent force constant). We finally discuss the connection between the elastic models and two well-established research fields of condensed-matter physics: point defects in crystals and solid-state diffusion.

cond-mat.soft↗

arXiv2005

A model for the generic alpha relaxation of viscous liquids

Dielectric measurements on molecular liquids just above the glass transition indicate that alpha relaxation is characterized by a generic high-frequency loss varying as $ω^{-1/2}$, whereas deviations from this come from one or more low-lying beta processes [Olsen et al, Phys. Rev. Lett. {\bf 86} (2001) 1271]. Assuming that long-wavelength fluctuations dominate the dynamics, a model for the dielectric alpha relaxation based on the simplest coupling between the density and dipole density fields is proposed here. The model, which is solved in second order perturbation theory in the Gaussian approximation, reproduces the generic features of alpha relaxation.

cond-mat.soft↗

arXiv2005

Solidity of viscous liquids. III. Alpha relaxation

It is suggested that the $ω^{-1/2}$ high-frequency decay of the alpha loss in highly viscous liquids, which appears to be generic, is a manifestation of a negative long-time tail as typically encountered in stochastic dynamics. The proposed mechanism requires that the coherent diffusion constant is much larger than estimated from the alpha relaxation time. This is justified by reference to the solidity of viscous liquids in an argument which, by utilizing the irrelevance of momentum conservation at high viscosity and introducing a center of mass diffusion constant, implies that at high viscosity the coherent diffusion constant is much larger than the incoherent diffusion constant.

cond-mat.soft↗

arXiv2004

Hopping models for ion conduction in noncrystals

Ion conduction in noncrystals (glasses, polymers, etc) has a number of properties in common. In fact, from a purely phenomenological point of view, these properties are even more widely observed: ion conduction behaves much like electronic conduction in disordered materials (e.g., amorphous semiconductors). These universalities are subject of much current interest, for instance interpreted in the context of simple hopping models. In the present paper we first discuss the temperature dependence of the dc conductivity in hopping models and the importance of the percolation phenomenon. Next, the experimental (quasi)universality of the ac conductivity is discussed. It is shown the random barrier model is able to reproduce the experimental finding that the response obeys time-temperature superposition, while at the same time a broad range of activation energies is involved in the conduction process. Again, percolation is the key to understanding what is going on. Finally, some open problems in the field are listed.

cond-mat.dis-nn↗

arXiv2004

A single-frequency test for one-parameter models of the linear thermo-visco-elastic response of glass-forming liquids

A master equation description of the inherent dynamics is used to calculate the frequency-dependent linear thermo-visco-elastic response functions of a glass-forming liquid. From the imaginary parts of the isobaric specific heat, isothermal bulk modulus, and isobaric thermal expansion coefficient, we define a quantity $Λ_{Tp}(ω)$ with the property that $Λ_{Tp}(ω)=1$ is equivalent to having a one-parameter description of the linear thermo-visco-elastic response. This provides an alternative to the well-known criterion based on the Prigogine-Defay ratio.

cond-mat.stat-mech↗

arXiv2003

Minimal model for beta relaxation in viscous liquids

Contrasts between beta relaxation in equilibrium viscous liquids and glasses are rationalized in terms of a double-well potential model with structure-dependent asymmetry, assuming structure is described by a single order parameter. The model is tested for tripropylene glycol where it accounts for the hysteresis of the dielectric beta loss peak frequency and magnitude during cooling and reheating through the glass transition.

cond-mat.soft↗

arXiv2003

Landscape equivalent of the shoving model

It is shown that the shoving model expression for the average relaxation time of viscous liquids follows largely from a classical "landscape" estimation of barrier heights from curvature at energy minima. The activation energy involves both instantaneous bulk and shear moduli, but the bulk modulus contributes less than 8% to the temperature dependence of the activation energy. This reflects the fact that the physics of the two models are closely related.

cond-mat.soft↗

arXiv2002

Is there a "native" band gap in ion conducting glasses?

It is suggested that the spectrum of ion site energies in glasses exhibits a band gap, establishing an analogy between ion conducting glasses and intrinsic semiconductors. This implies that ion conduction in glasses takes place via vacancies and interstitial ions (as in crystals).

cond-mat.dis-nn↗

arXiv2001

Hopping models and ac universality

Some general relations for hopping models are established. We proceed to discuss the universality of the ac conductivity which arises in the extreme disorder limit of the random barrier model. It is shown that the relevant dimension entering into the diffusion cluster approximation (DCA) is the harmonic (fracton) dimension of the diffusion cluster. The temperature scaling of the dimensionless frequency entering into the DCA is discussed. Finally, some open questions about ac universality are mentioned.

cond-mat.dis-nn↗

arXiv2001

Testing models for structural relaxation of viscous liquids by temperature jump experiments

Based on the Tool-Narayanaswami formalism for structural relaxation we propose an experiment which independent of the relaxation time distribution determines the structural relaxation rate by subtracting relaxations following two different temperature jumps. In particular, the experiment makes it possible to evaluate the relaxation rate immediately following a temperature jump - thus allowing one to distinguish the entropy model from others.

cond-mat.soft↗

arXiv2000

Time-temperature superposition in viscous liquids

Dielectric relaxation measurements on supercooled triphenyl phosphite show that at low temperatures time-temperature superposition (TTS) is accurately obeyed for the primary (alpha) relaxation process. Measurements on 6 other molecular liquids close to the calorimetric glass transition indicate that TTS is linked to an $ω^{-1/2}$ high-frequency decay of the alpha loss, while the loss peak width is nonuniversal.

cond-mat.soft↗

arXiv1999

Crossover to Potential Energy Landscape Dominated Dynamics in a Model Glass-forming Liquid

An equilibrated model glass-forming liquid is studied by mapping successive configurations produced by molecular dynamics simulation onto a time series of inherent structures (local minima in the potential energy). Using this ``inherent dynamics'' approach we find direct numerical evidence for the long held view that below a crossover temperature, $T_x$, the liquid's dynamics can be separated into (i) vibrations around inherent structures and (ii) transitions between inherent structures (M. Goldstein, J. Chem. Phys. {\bf 51}, 3728 (1969)), i.e., the dynamics become ``dominated'' by the potential energy landscape. In agreement with previous proposals, we find that $T_x$ is within the vicinity of the mode-coupling critical temperature $T_c$. We further find that at the lowest temperature simulated (close to $T_x$), transitions between inherent structures involve cooperative, string like rearrangements of groups of particles moving distances substantially smaller than the average interparticle distance.

cond-mat.soft↗

arXiv1999

Scaling and universality of AC conduction in disordered solids

Recent scaling results for the AC conductivity of ionic glasses by Roling et al. [Phys. Rev. Lett. vol 78, 2160 (1997)] and Sidebottom [Phys. Rev. Lett. vol 82, 3653 (1999)] are discussed. It is shown that Sidebottom's version of scaling is completely general. A new analytical approximation to the universal AC conductivity of hopping in the extreme disorder limit, the ``diffusion cluster approximation,'' is presented and compared to simulations and experiments.

cond-mat.dis-nn↗

arXiv1999

Beta-relaxation of non-polymeric liquids close to the glass transition

Dielectric beta-relaxation in a pyridine-toluene solution is studied close to the glass transition. In the equilibrium liquid state the beta loss peak frequency is not Arrhenius (as in the glass) but virtually temperature-independent, while the maximum loss is strongly temperature-dependent. Both loss peak frequency and maximum loss exhibit thermal hysteresis. A new annealing-state independent parameter involving loss and loss peak frequency is identified. This parameter has a simple Arrhenius temperature-dependence and is unaffected by the glass transition.

cond-mat.soft↗

arXiv1998

Solidity of Viscous Liquids

Recent NMR experiments on supercooled toluene and glycerol by Hinze and Bohmer show that small rotation angles dominate with only few large molecular rotations. These results are here interpreted by assuming that viscous liquids are solid-like on short length scales. A characteristic length, the "solidity length", separates solid-like behavior from liquid-like behavior.

cond-mat↗