TY - JOUR

T1 - Dielectric and shear mechanical relaxations in glass-forming liquids

T2 - A test of the Gemant-DiMarzio-Bishop model

AU - Niss, Kristine

AU - Jakobsen, Bo

AU - Olsen, Niels Boye

PY - 2005

Y1 - 2005

N2 - The Gemant-DiMarzio-Bishop model, which connects the frequency-dependent shear modulus to the frequency-dependent dielectric constant, is reviewed and a new consistent macroscopic formulation is derived. It is moreover shown that this version of the model can be tested without fitting parameters. The reformulated version of the model is analyzed and experimentally tested. It is demonstrated that the model has several nontrivial qualitative predictions: the existence of an elastic contribution to the high-frequency limit of the dielectric constant, a shift of the shear modulus loss peak frequency to higher frequencies compared with the loss peak frequency of the dielectric constant, a broader alpha peak, and a more pronounced beta peak in the shear modulus when compared with the dielectric constant. It is shown that these predictions generally agree with experimental findings and it is therefore suggested that the Gemant-DiMarzio-Bishop model is correct on a qualitative level. The quantitative agreement between the model and the data is on the other hand moderate to poor. It is discussed if a model-free comparison between the dielectric and shear mechanical relaxations is relevant, and it is concluded that the shear modulus should be compared with the rotational dielectric modulus, 1/(epsilon(omega)–n^2), which is extracted from the Gemant-DiMarzio-Bishop model, rather than to the dielectric susceptibility or the conventional dielectric modulus M=1/epsilon(omega)

AB - The Gemant-DiMarzio-Bishop model, which connects the frequency-dependent shear modulus to the frequency-dependent dielectric constant, is reviewed and a new consistent macroscopic formulation is derived. It is moreover shown that this version of the model can be tested without fitting parameters. The reformulated version of the model is analyzed and experimentally tested. It is demonstrated that the model has several nontrivial qualitative predictions: the existence of an elastic contribution to the high-frequency limit of the dielectric constant, a shift of the shear modulus loss peak frequency to higher frequencies compared with the loss peak frequency of the dielectric constant, a broader alpha peak, and a more pronounced beta peak in the shear modulus when compared with the dielectric constant. It is shown that these predictions generally agree with experimental findings and it is therefore suggested that the Gemant-DiMarzio-Bishop model is correct on a qualitative level. The quantitative agreement between the model and the data is on the other hand moderate to poor. It is discussed if a model-free comparison between the dielectric and shear mechanical relaxations is relevant, and it is concluded that the shear modulus should be compared with the rotational dielectric modulus, 1/(epsilon(omega)–n^2), which is extracted from the Gemant-DiMarzio-Bishop model, rather than to the dielectric susceptibility or the conventional dielectric modulus M=1/epsilon(omega)

U2 - 10.1063/1.2136886

DO - 10.1063/1.2136886

M3 - Journal article

SN - 0021-9606

VL - 123

SP - 234510

JO - Journal of Chemical Physics

JF - Journal of Chemical Physics

ER -