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Register a new userTheory of the highly viscous flow
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Authors
U. Buchenau
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The recent theoretical treatment of irreversible jumps between inherent states with a constant density in shear space is extended to a full theory, attributing the shear relaxation to structural Eshelby rearrangements involving the creation and annihilation of soft modes. The scheme explains the Kohlrausch exponent close to 1/2 and the connection to the low temperature glass anomalies. A continuity relation between the irreversible and the reversible Kohlrausch relaxation time distribution is derived. The full spectrum can be used in many ways, not only to describe shear relaxation data, but also to relate shear relaxation data to dielectric and bulk relaxation spectra, and to predict aging from shear relaxation data, as demonstrated for a very recent aging experiment.
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The recent Eshelby description of the highly viscous flow leads to the prediction of a factor of two different viscosities in stationary and alternating flow, in agreement with experimental evidence. The Kohlrausch barrier density increase with increasing barrier height finds a physical justification in the Adam-Gibbs increase of the number of structural alternatives of the Eshelby region with its increasing size. The new Ansatz allows to determine the number of atoms or molecules in the rearranging Eshelby domains from a combination of dynamic shear relaxation and calorimetric data.
The recent description of the highly viscous flow in terms of irreversible structural Eshelby rearrangements is extended to calculate the heat capacity of a glass former at a constant cooling rate through the glass transition. The result is compared to measured data from the literature, showing that the explanation works both for polymers and other glass formers.
Supplemental Material to ArXiv:1902.02746
We review a new theory of viscoelasticity of a glass-forming viscous liquid near and below the glass transition. In our model we assume that each point in the material has a specific viscosity, which varies randomly in space according to a fluctuating activation free energy. We include a Maxwellian elastic term and assume that the corresponding shear modulus fluctuates as well with the same distribution as that of the activation barriers. The model is solved in coherent-potential approximation (CPA), for which a derivation is given. The theory predicts an Arrhenius-type temperature dependence of the viscosity in the vanishing-frequency limit, independent of the distribution of the activation barriers. The theory implies that this activation energy is generally different from that of a diffusing particle with the same barrier-height distribution. If the distribution of activation barriers is assumed to have Gaussian form, the finite-frequency version of the theory describes well the typical low-temperature alpha relaxation peak of glasses. Beta relaxation can be included by adding another Gaussian with center at much lower energies than that responsible for the alpha relaxation. At high frequencies our theory reduces to the description of an elastic medium with spatially fluctuating elastic moduli (heterogeneous elasticity theory), which explains the occurrence of the boson-peak-related vibrational anomalies of glasses.
Atomic correlations in a simple liquid in steady-state flow under shear stress were studied by molecular dynamics simulation. The local atomic level strain was determined through the anisotropic pair-density function (PDF). The atomic level strain has a limited spatial extension whose range is dependent on the strain rate and extrapolates to zero at the critical strain rate. A failure event is identified with altering the local topology of atomic connectivity by exchanging bonds among neighboring atoms.
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