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Translational and rotational diffusion in supercooled orthoterphenyl close to the glass transition

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Zeitschrift für Physik B Condensed Matter

Abstract

Self diffusion coefficients in supercooled orthoterphenyl (OTP) have been determined down toD t =3·10−14 m2s−1 using a1H-NMR technique applying static field gradients up to 53T m−1 In a range of more than two decades theD t values agree with those of photochromic tracer molecules of the same size determined by forced Rayleigh scattering down to the glass transition temperatureT g . A change of mechanism is found for translational diffusion atT c ≈1.2T g whereD t is proportional to the inverse shear viscosityη −1 atT>T c butD t ∼η ξ with ξ=0.75 atT<T c . Rotational correlation times determined by2H-NMR stimulated echo techniques in deuterated OTP remain proportinal toη −1 down toT g . Our results are discussed in relation with mode coupling theory and with models of cooperative motion at the glass transition.

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References

  1. Angell, A.: J. Non-Cryst. Solids102, 205 (1988)

    Google Scholar 

  2. Angell, A.: J. Non-Cryst. Solids131–133, 13 (1991)

    Google Scholar 

  3. Rössler, E., Börner, K., Schulz, M., Taupitz, M.: J. Non-Cryst. Solids131–133, 99 (1991)

    Google Scholar 

  4. Rössler, E., Sillescu, H.: In: Material science and technology. Vol. 9: Glasses and amorphous materials, Zarzycki, J. (ed.), p. 573. Weinheim: Verlag Chemie 1991

    Google Scholar 

  5. Crank, J., Park, G.S.: Diffusion in polymers. London: Academic Press 1968

    Google Scholar 

  6. Ehlich, D., Sillescu, H.: Macromolecules23, 1600 (1990)

    Google Scholar 

  7. Götze, W.: In: Liquid, freezing and the glass transition. Levesque, D., Hansen, J.P., Zinn-Justin, J. (eds.). Amterdam, New York: Les Houches LI/Elsevier (to be published)

  8. Sjögren, L., Götze, W.: In: Springer Proceedings in Physics, Vol. 37, Richter, D., Dianoux, A.J., Petry, W., Teixeira, J. (eds.), p. 18. Berlin, Heidelberg, New York: Springer 1989

    Google Scholar 

  9. Götze, W., Sjögren, L.: J. Phys. C21, 3407 (1988)

    Google Scholar 

  10. Sjögren, L.: Z. Phys. B-Condensed Matter79, 5 (1990)

    Google Scholar 

  11. Mezei, F., Knaak, W., Farago, B.: Phys. Rev. Lett.58, 571 (1987)

    Google Scholar 

  12. Knaak, W., Mezei, F., Farago, B.: Europhys. Lett.7, 529 (1988)

    Google Scholar 

  13. Frick, B., Richter, D., Petry, W., Buchenau, U.: Z. Phys. B-Condensed Matter70, 73 (1988)

    Google Scholar 

  14. Petry, W., Bartsch, E., Fujara, F., Kiebel, M., Sillescu, H., Farago, B.: Z. Phys. B.-Condensed Matter83, 175 (1991)

    Google Scholar 

  15. Adam, G., Gibbs, J.H.: J. Chem. Phys.28, 373 (1965)

    Google Scholar 

  16. Fredrickson, G.H.: Annu. Rev. Phys. Chem.39, 149 (1988)

    Google Scholar 

  17. Cohen, M.T., Turnbull, D.: J. Chem. Phys.31, 1164 (1959)

    Google Scholar 

  18. Jäckle, J.: Rep. Prog. Phys.49, 171 (1986)

    Google Scholar 

  19. Tyrrell, H.J.V., Harris, K.R.: Diffusion in liquids. London: Butterworths 1984

    Google Scholar 

  20. McCall, D.W., Douglass, D.C., Falcone, D.R.: J. Chem. Phys.50, 3839 (1969)

    Google Scholar 

  21. Dries, Th., Fujara, F., Kiebel, M., Rössler, E., Sillescu, H.: J. Chem. Phys.88, 2139 (1988)

    Google Scholar 

  22. Schnauss, W., Fujara, F., Sillescu, H.: J. Chem. Phys. (in press)

  23. Bondi, A.: J. Phys. Chem.68, 441 (1964)

    Google Scholar 

  24. Lohfink, M., Sillescu, H.: Proceedings of the 1st Tohwa University, International Symposium, Fukuoka. Japan 4–8 November 1991. American Institute of Physics Conference Series (in press)

  25. Williams, G., Hains, P.J.: Chem. Phys. Lett.10, 58 (1971)

    Google Scholar 

  26. Williams, G., Shears, M.F.: J. Chem. Soc. Faraday69, 608 (1973)

    Google Scholar 

  27. Hyde, P.D., Evert, T.E., Ediger, M.D.: J. Chem. Phys.93, 2274 (1990)

    Google Scholar 

  28. Rössler, E., Börner, Tauchert, J., Taupitz, M., Pöschl, M.: Ber. Bunsenges. Physik. Chem.95, 1077 (1991)

    Google Scholar 

  29. Hinze, G.: (unpublished)

  30. Debus, O., Zimmermann, H., Bartsch, E., Fujara, F., Kiebel, M., Petry, W., Sillescu, H.: Chem. Phys. Lett.180, 271 (1991)

    Google Scholar 

  31. Tanner, J.E.: J. Chem Phys.52, 2523 (1970)

    Google Scholar 

  32. Kimmich, R., Unrath, W., Schnur, G., Rommel, E.: J. Magn. Reson91, 136 (1991)

    Google Scholar 

  33. Cukiermann, M., Lane, J.W., Uhlmann, D.R.: J. Chem. Phys.59, 3639 (1973)

    Google Scholar 

  34. Laughlin, W.T., Uhlmann, D.R.: J. Phys. Chem.76, 2317 (1972)

    Google Scholar 

  35. McLaughlin, E., Ubbelohde, A.R.: Trans. Faraday Soc.54, 1804 (1958)

    Google Scholar 

  36. Spiess, H.W.: J. Chem. Phys.72, 6755 (1980)

    Google Scholar 

  37. Fujara, F., Wefing, S., Spiess, H.W.: J. Chem Phys.84, 4579 (1986)

    Google Scholar 

  38. Fujara, F., Petry, W., Schnauss, W., Sillescu, H.: J. Chem. Phys.88, 792 (1988)

    Google Scholar 

  39. Geil, B., Fujara, F., Sillescu, H.: (to be published)

  40. Jeffrey, K. R.: Bull. Magn. Res3, 69 (1981)

    Google Scholar 

  41. Wefing, S.: Dissertation, Universität Mainz 1987

  42. Wefing, S., Spiess, H.W.: J. Chem. Phys.89, 1219 (1988)

    Google Scholar 

  43. Diehl, R.M., Fujara, F., Sillescu, H.: Europhys. Lett.13, 257 (1990)

    Google Scholar 

  44. Lohfink, M.: Diplomarbeit, Universität Mainz 1988, Dissertation, Universität Mainz 1991

  45. Heller, H.G., Langau, J.R.: J. Chem. Soc. Perkin Trans. 21981, 341

  46. Jones, P., Darcy, P., Attard, G.S., Jones, W.J., Williams, G.: Mol. Phys.67, 1053 (1989)

    Google Scholar 

  47. Böttcher, C.J.F., Bordewijk, P.: Theory of electric polarization. Vol. II. Amsterdam: Elsevier 1978

    Google Scholar 

  48. Lindsay, C.P., Patterson, G.D.: J. Chem. Phys.73, 3348 (1980)

    Google Scholar 

  49. Fytas, G., Wang, C.H., Lilge, D., Dorfmüller, T.H.: J. Chem. Phys.75, 4274 (1981)

    Google Scholar 

  50. Beevers, M., Crossley, Garringtong, D.,Williams, G.: J. Chem. Soc. Faraday Trans 273, 458 (1977)

    Google Scholar 

  51. Johari, G.P., Goldstein, M.: J. Chem. Phys.53, 2372 (1970)

    Google Scholar 

  52. Johari, G.P.: Lecture Notes in Physics. Vol. 277, Dorfmüller, T., William, G. (eds.) p. 90–112. Berlin, Heidelberg, New York: Springer

  53. Rössler, E., Schnauss W.: Chem. Phys. Lett.170, 315 (1990)

    Google Scholar 

  54. Bartsch, E., Debus, O., Fujara, F., Kiebel, M., Sillescu, H., Petry, W.: Ber. Bunsenges. Phys. Chem.95, 1146 (1991)

    Google Scholar 

  55. Debus, O., Zimmermann, H., Bartsch, E., Fujara, E., Kiebel, M., Petry, W.: Chem. Phys. Lett.180, 271 (1991)

    Google Scholar 

  56. Birge, N.O., Nagel, S.R.: Phys. Rev. Lett.54, 2674 (1985)

    Google Scholar 

  57. Dixon, P.K., Nagel, S.R.: Phys. Rev. Lett.61, 341 (1988)

    Google Scholar 

  58. Götze, W., Latz, A.: J. Phys. G.1, 4169 (1989)

    Google Scholar 

  59. Götze, W., Sjögren, L.: Z. Phys. B-Condensed Matter65, 415 (1987), J. Phys. C21, 3407 (1988)

    Google Scholar 

  60. Fujita, H.: Fortschr. Hochpolym. Forsch.3, 1 (1961)

    Google Scholar 

  61. Vrentas, J.S., Duda, J.L.: J. Chem. Sci. (Polym. Phys. Ed.)15, 403 (1977)

    Google Scholar 

  62. Vrentas, J.S., Duda, J.L., Hou, A.C.: J. Appl. Polym. Sci.31, 739 (1986)

    Google Scholar 

  63. Coughlin, Ch.S., Mauritz, K.A., Storey, R.F.: Macromolecules24, 1526 (1991) and references therein

    Google Scholar 

  64. Flynn, C.P.: Point defects and diffusion. Oxford: Clarendon 1972

    Google Scholar 

  65. Huber, D.L.: J. Chem. Phys.78, 2530 (1973)

    Google Scholar 

  66. Grünewald, M., Pohlmann, B., Movaghar, B., Würz, D.: Philos. Mag. B.49, 341 (1984)

    Google Scholar 

  67. Bässler, H.: Phys. Rev. Lett.58, 767 (1987)

    Google Scholar 

  68. Frauenfelder, H.: Helv. Phys. Acta57, 165 (1984)

    Google Scholar 

  69. Klinger, M.I.: Phys. Rep.165, 275 (1988)

    Google Scholar 

  70. Funke, K.: Ber. Bunsenges. Phys. Chem.95, 955 (1991)

    Google Scholar 

  71. Kivelson, D., Miles, D.: J. Chem. Phys.88, 1925 (1988)

    Google Scholar 

  72. Kivelson, D., Kivelson, S.A.: J. Chem. Phys.90, 4464 (1989)

    Google Scholar 

  73. Kivelson, D.: J. Chem. Phys.95, 709 (1991)

    Google Scholar 

  74. Antonietti, M.: (Private communication)

  75. Donth, E.J.: J. Non-Cryst. Solids53, 325 (1982),204, 131 (1991)

    Google Scholar 

  76. Donth, E.J.: Glasübergang. Berlin: Akademie Verlag 1981

    Google Scholar 

  77. Endom, L., Hertz, H.G., Thul, B., Zeidler, M.D.: Ber. Bunsenges. Phys. Chem.72, 1008 (1967)

    Google Scholar 

  78. Rössler, E.: Phys. Rev. Lett.65, 1595 (1990)

    Google Scholar 

  79. Fytas, G., Rizos, A., Floudas, G., Lodge, T.P.: J. Chem. Phys.93, 5096 (1990)

    Google Scholar 

  80. Richter, D., Zorn, R., Farago, B., Frick, B., Fetters, L.J.: Phys. Rev. Lett.68, 71 (1992)

    Google Scholar 

  81. Fischer, E.W., Donth, E., Steffen, W.: Phys. Rev. Lett.68, 2344 (1992)

    Google Scholar 

  82. Steffen, W., Patkowski, A., Meier, G., Fischer, E.W.: J. Chem. Phys.96, 4171 (1992)

    Google Scholar 

  83. Fischer E.W., Becker, Ch., Hagenah, J.-U, Meier, G.: Prog. Coll. Polym. Sci.80, 198 (1989)

    Google Scholar 

  84. Butler, S., Harrowell, P.: J. Chem. Phys.95, 4454 (1991)

    Google Scholar 

  85. Adachi, K.: Macromolecules23, 1816 (1990)

    Google Scholar 

  86. Matsuoka, S., Quan: J. Non-Cryst. Solids293 131 (1991)

    Google Scholar 

  87. Stillinger, F.H.: J. Chem. Phys.89, 6461 (1988)

    Google Scholar 

  88. Schmidt-Rohr, K., Spiess, H.W.: Phys. Rev. Lett.66, 3020 (1991)

    Google Scholar 

  89. Schnauss, W., Fujara, F., Hartmann, K., Sillescu, H.: Chem. Phys. Lett.166, 381–384 (1990)

    Google Scholar 

  90. Diezemann, G., Schirmacher, W.: J. Phys. G2, 6681 (1990)

    Google Scholar 

  91. Spiess, H.W.: Chem. Rev.91, 1321 (1991)

    Google Scholar 

  92. Heuberger, G., Sillescu, H.: Polymer Preprints33, 105 (1992)

    Google Scholar 

  93. Gerharz, B., Meier, G., Fischer, E.W.: J. Chem. Phys.92, 7110 (1990)

    Google Scholar 

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Authors and Affiliations

  1. Institut für Physikalische Chemie, Universität Mainz, Jakob-Welder-Weg 15, W-6500, Mainz, Federal Republic of Germany

    F. Fujara, B. Geil & H. Sillescu

  2. Sektion Physik, Universität Leipzig, Linnéstrasse 5, O-7066, Leipzig, Federal Republic of Germany

    G. Fleischer

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  1. F. Fujara
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  2. B. Geil
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  3. H. Sillescu
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  4. G. Fleischer
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Fujara, F., Geil, B., Sillescu, H. et al. Translational and rotational diffusion in supercooled orthoterphenyl close to the glass transition. Z. Physik B - Condensed Matter 88, 195–204 (1992). https://doi.org/10.1007/BF01323572

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