A resolution for the enigma of a liquid's configurational entropy-molecular kinetics relation

Journal of Chemical Physics

Volumn 112, Issue 20, 2000, Pages 8958-8969

  Johari, G P ^a  

^a MCMASTER UNIVERSITY   (Canada)

Author keywords

[No Author keywords available]

Indexed keywords

EID: 0000744308     PISSN: 00219606     EISSN: None     Source Type: Journal    
DOI: 10.1063/1.481509     Document Type: Article

References (94)

1. M. H. Cohen and D. Turnbull, J. Chem. Phys. 31, 1164 (1959); 34, 120 (1961); 52, 3038 (1970).
2. M. H. Cohen and D. Turnbull, J. Chem. Phys. 31, 1164 (1959); 34, 120 (1961); 52, 3038 (1970).
3. M. H. Cohen and D. Turnbull, J. Chem. Phys. 31, 1164 (1959); 34, 120 (1961); 52, 3038 (1970).
4. M. H. Cohen and G. H. Grest, Phys. Rev. B 20, 1077 (1979); 21, 4113 (1980).
5. M. H. Cohen and G. H. Grest, Phys. Rev. B 20, 1077 (1979); 21, 4113 (1980).
6. J. H. Gibbs and E. A. DiMarzio, J. Chem. Phys. 28, 373 (1958).
7. G. Adam and J. W. Gibbs, J. Chem. Phys. 43, 139 (1965).
8. G. P. Johari and E. Whalley, Faraday Symp. Chem. Soc. 6, 23 (1972).
9. S. Takahara, O. Yamamuro, and H. Suga, J. Non-Cryst. Solids 171, 259 (1994).
10. G. P. Johari and M. Goldstein, J. Chem. Phys. 53, 2372 (1970); 55, 4245 (1971).
11. G. P. Johari and M. Goldstein, J. Chem. Phys. 53, 2372 (1970); 55, 4245 (1971).
12. G. P. Johari, J. Chem. Phys. 58, 1766 (1973).
13. g, /T) plots, has discussed these in a monograph, S. Nemilov, Thermodynamics and Kinetic Aspects of the Vitreous State (CRC, Boca Raton, 1995).
14. g, /T) plots, has discussed these in a monograph, S. Nemilov, Thermodynamics and Kinetic Aspects of the Vitreous State (CRC, Boca Raton, 1995).
15. g, /T) plots, has discussed these in a monograph, S. Nemilov, Thermodynamics and Kinetic Aspects of the Vitreous State (CRC, Boca Raton, 1995).
16. K. Ito, C. T. Moynihan, and C. A. Angell, Nature (London) 398, 492 (1999).
17. U. Mohanty, Adv. Chem. Phys. 89, 89 (1994).
18. U. Mohanty, I. Oppenheim, and C. H. Taubes, Science 266, 425 (1994).
19. K. L. Ngai, J. Phys. Chem. 103, 5895 (1999); J. Chem. Phys. 111, 3639 (1999).
20. K. L. Ngai, J. Phys. Chem. 103, 5895 (1999); J. Chem. Phys. 111, 3639 (1999).
21. C. M. Roland, P. G. Santangelo, and K. L. Ngai, J. Chem. Phys. 111, 5593 (1999).
22. K. L. Ngai and O. Yamamuro, J. Chem. Phys. 111, 10403 (1999).
23. M. Goldstein, J. Chem. Phys. 51, 3728 (1969).
24. G. P. Johari, J. Mol. Struct. 520, 249 (1999); J. Phys. Chem. 103, 11036 (1999).
25. G. P. Johari, J. Mol. Struct. 520, 249 (1999); J. Phys. Chem. 103, 11036 (1999).
26. J. H. Magill, J. Chem. Phys. 47, 2802 (1967); see also D. J. Plazek, J. H. Magill, I. Echeverria, and I.-C. Chay, ibid. 110, 10445 (1999) for correct identification of the material.
27. J. H. Magill, J. Chem. Phys. 47, 2802 (1967); see also D. J. Plazek, J. H. Magill, I. Echeverria, and I.-C. Chay, ibid. 110, 10445 (1999) for correct identification of the material.
28. 2, etc., differ significantly from the corresponding plots of organic liquids. They concluded that categorization of liquids in such a simple manner tends to "...obscure certain features of the available experimental data which are important for understanding the process of viscous flow." Despite that, such plots are used extensively to characterize liquids as "fragile and strong," (Refs. 9 and 10) in place of "long and short," the century-old terms used by glass-makers to refer qualitatively to the duration, (i) in which a glass-maker or the machine should shape an object from its melt, and (ii) needed for annealing out the internal stresses from the finished object. The viscosity of a "short" or "fragile" glass is more sensitive to the temperature change, or its temperature dependence is highly non-Arrhenius, than that of a "long" or "strong" glass.
29. See for a review, V. P. Privalko, J. Phys. Chem. 84, 3307 (1980).
30. I. M. Hodge, J. Non-Cryst. Solids 169, 211 (1994), and references therein.
31. I. M. Hodge, J. Res. Natl. Inst. Stand. Technol. 102, 195 (1997), and references therein.
32. I. M. Hodge and J. M. O'Reilly, J. Phys. Chem. B 103, 4171 (1999).
33. G. W. Scherer, J. Am. Ceram. Soc. 67, 504 (1984).
34. S. Takahara, O. Yamamuro, and T. Matsuo, J. Phys. Chem. 99, 9589 (1995).
35. O. Yamamuro, I. Tsukushi, A. Lindquist, S. Takahara, M. Ishikawa, and T. Matsuo, J. Phys. Chem. B 102, 1605 (1998).
36. R. Richert and C. A. Angell, J. Chem. Phys. 108, 9016 (1998).
37. W. Kauzmann, Chem. Rev. 43, 219 (1948).
38. G. P. Johari, Ann. (N.Y.) Acad. Sci. 279, 117 (1976).
39. M. Goldstein, J. Chem. Phys. 64, 4767 (1976); Ann. (N.Y.) Acad. Sci. 279, 68 (1976).
40. M. Goldstein, J. Chem. Phys. 64, 4767 (1976); Ann. (N.Y.) Acad. Sci. 279, 68 (1976).
41. P. D. Gujrati and M. Goldstein, J. Phys. Chem. 84, 859 (1980).
42. G. P. Johari, Ann. (N.Y.) Acad. Sci. 279, 102 (1976); Philos. Mag. B 41, 41 (1981).
43. G. P. Johari, Ann. (N.Y.) Acad. Sci. 279, 102 (1976); Philos. Mag. B 41, 41 (1981).
44. R. J. Greet and D. Turnbull, J. Chem. Phys. 47, 2185 (1967).
45. M. Goldstein, J. Chem. Phys. 67, 2246 (1977).
46. G. P. Johari, J. Chem. Phys. (in press).
47. K. L. Ngai, J. Chem. Phys. 111, 3639 (1999).
48. T.-P. Liau and H. Morawetz, Macromolecules 13, 1228 (1980).
49. H. Vogel, Phys. Z. 22, 645 (1921).
50. G. S. Fulcher, J. Am. Ceram. Soc. 8, 339 (1923).
51. G. Tamman and W. Hesse, Z. Anorg. Allg. Chem. 156, 245 (1926).
52. F. Stickel, E. W. Fischer, and R. Richert, J. Chem. Phys. 102, 6251 (1995); 104, 2043 (1996). Note that the three regions similar to those described by the authors were also noted in the viscosity data of tri-α- naphthylbenzene by Plazek and Magill [J. Chem. Phys. 49, 3678 (1968)] and for several liquids by Laughlin and Uhlmann [ J. Phys. Chem. 76, 2317 (1972)]. In a recent paper, K. L. Ngai, J. H. Magill, and D. J. Plazek, J. Chem. Phys. 112, 1887 (2000), have fitted the temperature dependence of the viscosity of tri-α-naphthylbenzene into three relaxation regions in a manner similar to that used by Stickel et al., and found that the viscosity data of tri-α-naphthylbenzene can not be fitted to a Vogel-Fulcher- Tamman equation with a single set of parameters over the entire temperature range. This may not be so surprising because the mechanism for viscous flow becomes gradually altered as heterogeneity in the molecular rearrangement develops on cooling a liquid and the α-relaxation process gains importance. In this view, the above-mentioned three regions would not, strictly speaking, correspond to a single transport mechanism in the entire temperature range.
53. F. Stickel, E. W. Fischer, and R. Richert, J. Chem. Phys. 102, 6251 (1995); 104, 2043 (1996). Note that the three regions similar to those described by the authors were also noted in the viscosity data of tri-α- naphthylbenzene by Plazek and Magill [J. Chem. Phys. 49, 3678 (1968)] and for several liquids by Laughlin and Uhlmann [ J. Phys. Chem. 76, 2317 (1972)]. In a recent paper, K. L. Ngai, J. H. Magill, and D. J. Plazek, J. Chem. Phys. 112, 1887 (2000), have fitted the temperature dependence of the viscosity of tri-α-naphthylbenzene into three relaxation regions in a manner similar to that used by Stickel et al., and found that the viscosity data of tri-α-naphthylbenzene can not be fitted to a Vogel-Fulcher- Tamman equation with a single set of parameters over the entire temperature range. This may not be so surprising because the mechanism for viscous flow becomes gradually altered as heterogeneity in the molecular rearrangement develops on cooling a liquid and the α-relaxation process gains importance. In this view, the above-mentioned three regions would not, strictly speaking, correspond to a single transport mechanism in the entire temperature range.
54. F. Stickel, E. W. Fischer, and R. Richert, J. Chem. Phys. 102, 6251 (1995); 104, 2043 (1996). Note that the three regions similar to those described by the authors were also noted in the viscosity data of tri-α-naphthylbenzene by Plazek and Magill [J. Chem. Phys. 49, 3678 (1968)] and for several liquids by Laughlin and Uhlmann [ J. Phys. Chem. 76, 2317 (1972)]. In a recent paper, K. L. Ngai, J. H. Magill, and D. J. Plazek, J. Chem. Phys. 112, 1887 (2000), have fitted the temperature dependence of the viscosity of tri-α-naphthylbenzene into three relaxation regions in a manner similar to that used by Stickel et al., and found that the viscosity data of tri-α-naphthylbenzene can not be fitted to a Vogel-Fulcher- Tamman equation with a single set of parameters over the entire temperature range. This may not be so surprising because the mechanism for viscous flow becomes gradually altered as heterogeneity in the molecular rearrangement develops on cooling a liquid and the α-relaxation process gains importance. In this view, the above-mentioned three regions would not, strictly speaking, correspond to a single transport mechanism in the entire temperature range.
55. F. Stickel, E. W. Fischer, and R. Richert, J. Chem. Phys. 102, 6251 (1995); 104, 2043 (1996). Note that the three regions similar to those described by the authors were also noted in the viscosity data of tri-α- naphthylbenzene by Plazek and Magill [J. Chem. Phys. 49, 3678 (1968)] and for several liquids by Laughlin and Uhlmann [ J. Phys. Chem. 76, 2317 (1972)]. In a recent paper, K. L. Ngai, J. H. Magill, and D. J. Plazek, J. Chem. Phys. 112, 1887 (2000), have fitted the temperature dependence of the viscosity of tri-α-naphthylbenzene into three relaxation regions in a manner similar to that used by Stickel et al., and found that the viscosity data of tri-α-naphthylbenzene can not be fitted to a Vogel-Fulcher- Tamman equation with a single set of parameters over the entire temperature range. This may not be so surprising because the mechanism for viscous flow becomes gradually altered as heterogeneity in the molecular rearrangement develops on cooling a liquid and the α-relaxation process gains importance. In this view, the above-mentioned three regions would not, strictly speaking, correspond to a single transport mechanism in the entire temperature range.
56. F. Stickel, E. W. Fischer, and R. Richert, J. Chem. Phys. 102, 6251 (1995); 104, 2043 (1996). Note that the three regions similar to those described by the authors were also noted in the viscosity data of tri-α- naphthylbenzene by Plazek and Magill [J. Chem. Phys. 49, 3678 (1968)] and for several liquids by Laughlin and Uhlmann [ J. Phys. Chem. 76, 2317 (1972)]. In a recent paper, K. L. Ngai, J. H. Magill, and D. J. Plazek, J. Chem. Phys. 112, 1887 (2000), have fitted the temperature dependence of the viscosity of tri-α-naphthylbenzene into three relaxation regions in a manner similar to that used by Stickel et al., and found that the viscosity data of tri-α-naphthylbenzene can not be fitted to a Vogel-Fulcher-Tamman equation with a single set of parameters over the entire temperature range. This may not be so surprising because the mechanism for viscous flow becomes gradually altered as heterogeneity in the molecular rearrangement develops on cooling a liquid and the α-relaxation process gains importance. In this view, the above-mentioned three regions would not, strictly speaking, correspond to a single transport mechanism in the entire temperature range.
57. M. Mizukami, K. Kobashi, M. Hanaya, and M. Oguni, J. Phys. Chem. 103, 4078 (1999).
58. K. Pathmanathan and G. P. Johari, Philos. Mag. B 62, 225 (1990).
59. P. Lunkenheimer, U. Schneider, R. Brand, and A. Loidl, Slow Dynamics in Complex Systems, Eighth Tohwa University International Symposium, edited by M. Tokuyama and I. Oppenheim (AIP, Woodbury, New York, 1999), p. 433.
60. A. Kudlik, S. Benkhof, T. Blochowicz, C. Tschirwitz, and E. Rossler, J. Mol. Struct. 479, 201 (1999).
61. S. S. Chang and A. B. Bestul, J. Chem. Phys. 56, 503 (1972).
62. J. G. Berberian and R. H. Cole, J. Chem. Phys. 84, 6921 (1986).
63. C. L. Jackson and G. B. McKenna, J. Non-Cryst. Solids 131-133, 211 (1991); Chem. Mater. 8, 2128 (1996).
64. C. L. Jackson and G. B. McKenna, J. Non-Cryst. Solids 131-133, 211 (1991); Chem. Mater. 8, 2128 (1996).
65. M. Arndt, R. Stannarius, W. Gorbatschow, and F. Kremer, Phys. Rev. E 54, 5377 (1996).
66. K. L. Ngai, J. Phys.: Condens. Matter 11, A119 (1999).
67. K. Takeda, O. Yamamuro, and H. Suga, J. Phys. Chem. Solids 52, 607 (1991).
68. K. Takeda, O. Yamamuro, and H. Suga, J. Phys. Chem. 99, 1602 (1995).
69. M. Sugisaki, K. Adachi, H. Suga, and S. Seki, Bull. Chem. Soc. Jpn. 41, 593 (1968).
70. D. R. Douslin and H. M. Huffman, J. Am. Chem. Soc. 68, 1704 (1946).
71. H. L. Finke and J. F. Messerly, J. Chem. Thermodyn. 5, 2447 (1973).
72. K. Kishimoto, H. Suga, and S. Seki, Bull. Chem. Soc. Jpn. 46, 3020 (1973).
73. T. Hikima, M. Hanaya, and M. Oguni, Solid State Commun. 93, 713 (1995). I should like to thank Professor M. Oguni for providing some of the heat capacity data for calculations.
74. I. Tsukushi, O. Yamamuro, T. Ohta, T. Matsuo, H. Nakano, and Y. Shirota, J. Phys.: Condens. Matter 8, 245 (1996).
75. H. Fujimori and M. Oguni, J. Chem. Thermodyn. 26, 367 (1994).
76. S. S. Chang and A. B. Bestul, J. Chem. Phys. 40, 3731 (1964).
77. T. Hikima, N. Okamoto, M. Hanaya, and M. Oguni, J. Chem. Thermodyn. 30, 509 (1998).
78. O. Haida, H. Suga, and S. Seki, J. Chem. Thermodyn. 9, 1133 (1977).
79. K. Takeda, O. Yamamuro, I. Tsukushi, T. Matsuo, and H. Suga, J. Mol. Struct. 479, 227 (1999).
80. J. F. Counsell, E. B. Lees, and J. F. Martin, J. Chem. Soc. A 1968, 1819.
81. G. E. Gibson and W. F. Giauque, J. Am. Chem. Soc. 45, 93 (1923).
82. J. P. McCullough, H. L. Finke, D. W. Scott, R. E. Pennington, M. E. Gross, J. F. Messerly, and G. Waddington, J. Am. Chem. Soc. 80, 4786 (1958).
83. D. W. Scott, J. P. McCullough, J. F. Messerly, R. E. Pennington, I. A. Hessenlop, H. L. Finke, and G. Waddington, J. Am. Chem. Soc, 80, 55 (1958).
84. J. F. Messerly, H. L. Finke, and S. S. Todd, J. Chem. Thermodyn. 6, 635 (1974).
85. T. Hikima, M. Hanaya, and M. Oguni, Solid State Commun. 93, 713 (1995), I am grateful to Professor M. Oguni and Dr. K. L. Ngai for providing some of the heat capacity data.
86. H. Hikawa, M. Oguni, and H. Suga, J. Non-Cryst. Solids 101, 90 (1988).
87. S. S. Chang, J. A. Horman, and A. B. Bestul, J. Res. Natl. Bur. Stand., Sect. A 71, 293 (1967).
88. G. S. Parks, S. B. Thomas, and D. Light, J. Chem. Phys. 4, 66 (1936).
89. H. Fujimori, M. Mizukami, and M. Oguni, J. Non-Cryst. Solids 204, 38 (1996).
90. J. E. Kunzler and W. F. Gaiuque, J. Am. Chem. Soc. 74, 797 (1952).
91. J. C. Southard, J. Am. Chem. Soc. 63, 3147 (1941).
92. S. S. Chang and A. B. Bestul, J. Chem. Thermodyn. 6, 325 (1974).
93. S. Matsuoka, J. Res. Natl. Inst. Stand. Technol. 102, 213 (1997), see also Relaxation Phenomena in Polymers (Hanser, New York, 1992).
94. S. Matsuoka, J. Res. Natl. Inst. Stand. Technol. 102, 213 (1997), see also Relaxation Phenomena in Polymers (Hanser, New York, 1992).