TY - JOUR

T1 - Evaluation of the Dyre shoving model using dynamic data near the glass temperature

AU - Xu, Ben

AU - McKenna, Gregory B.

N1 - Funding Information:
The authors are grateful to the Office of Naval Research (ONR) under Project No. N00014–06-1–0922 and the John R. Bradford endowment at Texas Tech University for partial support of this work. We also thank H. H. Winter for providing access to IRIS Software.

PY - 2011/3/28

Y1 - 2011/3/28

N2 - The temperature dependence of the dynamics of glass-forming systems remains an important fundamental problem in glass physics. Here we use literature data [S. A. Hutcheson and G. B. McKenna, J. Chem. Phys. 129, 074502 (2008)] reanalyzed with the Baumgrtel-Schausberger-Winter (BSW) [M. Baumgrtel, A. Schausberger, and H. H. Winter, Rheol. Acta 29, 400 (1990); M. Baumgrtel and H. H. Winter, ibid. 28, 511 (1989); M. Baumgrtel and H. H. Winter, J. Non-Newtonian Fluid Mech. 44, 15 (1992)] model of complex fluid dynamics to evaluate the Dyre shoving model [J. C. Dyre, N. B. Olsen, and T. Christensen, Phys. Rev. B 53, 2171 (1996); J. C. Dyre, Rev. Mod. Phys. 78, 953 (2006)] that relates the temperature dependence of viscosity to the infinite-frequency shear modulus and its temperature dependence. In Dyres model, the free-energy barrier for a flow event is attributed to the work done in shoving aside the surrounding molecules; the free-energy barrier is proportional to the glassy modulus, which increases as the temperature decreases. In the present work, the glassy modulus was obtained by the extrapolation to zero time or infinite frequency of the Kohlrausch-Williams-Watts (KWW) [G. Williams and D. C. Watts, Trans. Faraday Soc. 66, 80 (1970); F. Kolrausch, Pogg. Ann. Phys. 12, 393 (1847)] and BSW [M. Baumgrtel, A. Schausberger, and H. H. Winter, Rheol. Acta 29, 400 (1990); M. Baumgrtel and H. H. Winter, ibid. 28, 511 (1989); M. Baumgrtel and H. H. Winter, J. Non-Newtonian Fluid Mech. 44, 15 (1992)] functions to experimental data for m-toluidine and sucrose benzoate. It was found that the glassy modulus obtained from the KWW function for m-toluidine and sucrose benzoate [S. A. Hutcheson and G. B. McKenna, J. Chem. Phys. 129, 074502 (2008)] provides a consistent picture of the temperature-dependent dynamics within the framework of the shoving model. A similar analysis using a BSW description of the dynamics provides consistency for the sucrose benzoate but not for the m-toluidine.

AB - The temperature dependence of the dynamics of glass-forming systems remains an important fundamental problem in glass physics. Here we use literature data [S. A. Hutcheson and G. B. McKenna, J. Chem. Phys. 129, 074502 (2008)] reanalyzed with the Baumgrtel-Schausberger-Winter (BSW) [M. Baumgrtel, A. Schausberger, and H. H. Winter, Rheol. Acta 29, 400 (1990); M. Baumgrtel and H. H. Winter, ibid. 28, 511 (1989); M. Baumgrtel and H. H. Winter, J. Non-Newtonian Fluid Mech. 44, 15 (1992)] model of complex fluid dynamics to evaluate the Dyre shoving model [J. C. Dyre, N. B. Olsen, and T. Christensen, Phys. Rev. B 53, 2171 (1996); J. C. Dyre, Rev. Mod. Phys. 78, 953 (2006)] that relates the temperature dependence of viscosity to the infinite-frequency shear modulus and its temperature dependence. In Dyres model, the free-energy barrier for a flow event is attributed to the work done in shoving aside the surrounding molecules; the free-energy barrier is proportional to the glassy modulus, which increases as the temperature decreases. In the present work, the glassy modulus was obtained by the extrapolation to zero time or infinite frequency of the Kohlrausch-Williams-Watts (KWW) [G. Williams and D. C. Watts, Trans. Faraday Soc. 66, 80 (1970); F. Kolrausch, Pogg. Ann. Phys. 12, 393 (1847)] and BSW [M. Baumgrtel, A. Schausberger, and H. H. Winter, Rheol. Acta 29, 400 (1990); M. Baumgrtel and H. H. Winter, ibid. 28, 511 (1989); M. Baumgrtel and H. H. Winter, J. Non-Newtonian Fluid Mech. 44, 15 (1992)] functions to experimental data for m-toluidine and sucrose benzoate. It was found that the glassy modulus obtained from the KWW function for m-toluidine and sucrose benzoate [S. A. Hutcheson and G. B. McKenna, J. Chem. Phys. 129, 074502 (2008)] provides a consistent picture of the temperature-dependent dynamics within the framework of the shoving model. A similar analysis using a BSW description of the dynamics provides consistency for the sucrose benzoate but not for the m-toluidine.

UR - http://www.scopus.com/inward/record.url?scp=79953327326&partnerID=8YFLogxK

U2 - 10.1063/1.3567092

DO - 10.1063/1.3567092

M3 - Article

C2 - 21456698

AN - SCOPUS:79953327326

SN - 0021-9606

VL - 134

JO - The Journal of Chemical Physics

JF - The Journal of Chemical Physics

IS - 12

M1 - 124902

ER -