COOPERATIVE MOTION IN FRAGILE LIQUIDS NEAR THE GLASS-TRANSITION - PROBE REORIENTATION IN O-TERPHENYL AND POLYSTYRENE

被引:53
作者
BLACKBURN, FR [1 ]
CICERONE, MT [1 ]
HIETPAS, G [1 ]
WAGNER, PA [1 ]
EDIGER, MD [1 ]
机构
[1] UNIV WISCONSIN,DEPT CHEM,MADISON,WI 53706
关键词
D O I
10.1016/0022-3093(94)90444-8
中图分类号
TQ174 [陶瓷工业]; TB3 [工程材料学];
学科分类号
0805 ; 080502 ;
摘要
Reorientational relaxation measurements of dilute rigid probes in o-terphenyl and polystyrene are reported. In each matrix, the results span more than 13 decades in time and extend to below the conventional glass transition temperature. The temperature dependence of the observed rotation times is roughly proportional to viscosity divided by temperature, as predicted by the Debye-Stokes-Einstein equation. Consistent with previous work on o-terphenyl [F. Fujara, B. Geil, H. Sillescu and G. Fleischer, Z. Phys. B88 (1992) 195], it is observed that probe rotational motion has a stronger temperature dependence than probe translational diffusion at low temperatures. Using translational diffusion results from the literature, it is shown for the first time that this is also true in a polymeric glass former. These results are inconsistent with several proposed models of cooperativity near the glass transition.
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收藏
页码:256 / 264
页数:9
相关论文
共 30 条
[1]   ON TEMPERATURE DEPENDENCE OF COOPERATIVE RELAXATION PROPERTIES IN GLASS-FORMING LIQUIDS [J].
ADAM, G ;
GIBBS, JH .
JOURNAL OF CHEMICAL PHYSICS, 1965, 43 (01) :139-&
[2]   STUDY OF THE THERMAL POLYMERIZATION OF STYRENE BY DEPOLARIZED RAYLEIGH LIGHT-SCATTERING SPECTROSCOPY [J].
ALMS, GR ;
PATTERSON, GD ;
STEVENS, JR .
JOURNAL OF CHEMICAL PHYSICS, 1979, 70 (05) :2145-2154
[3]  
ANDERSON JE, 1972, FARADAY S CHEM SOC, V6, P82
[4]   AN INTERPRETATION OF THE BIFURCATION OF ORIENTATIONAL RELAXATION PROCESSES IN A SUPERCOOLED LIQUID [J].
BAGCHI, B ;
CHANDRA, A ;
RICE, SA .
JOURNAL OF CHEMICAL PHYSICS, 1990, 93 (12) :8991-9001
[5]   MOLECULAR-DYNAMICS SIMULATIONS OF SUPERCOOLED LIQUIDS NEAR THE GLASS-TRANSITION [J].
BARRAT, JL ;
KLEIN, ML .
ANNUAL REVIEW OF PHYSICAL CHEMISTRY, 1991, 42 :23-53
[6]   MOLECULAR-DYNAMICS OF VISCOUS-LIQUIDS - COMPARISON OF DIELECTRIC AND KERR-EFFECT RELAXATION FOR TRITOLYL PHOSPHATE, ORTHO-TERPHENYL AND THEIR MIXTURES [J].
BEEVERS, MS ;
CROSSLEY, J ;
GARRINGTON, DC ;
WILLIAMS, G .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS II, 1977, 73 :458-470
[7]   THE SOLUTE SIZE EFFECT IN ROTATIONAL DIFFUSION EXPERIMENTS - A TEST OF MICROSCOPIC FRICTION THEORIES [J].
BENAMOTZ, D ;
DRAKE, JM .
JOURNAL OF CHEMICAL PHYSICS, 1988, 89 (02) :1019-1029
[8]   TRANSLATIONAL AND ROTATIONAL MOLECULAR-MOTION IN SUPERCOOLED LIQUIDS STUDIED BY NMR AND FORCED RAYLEIGH-SCATTERING [J].
CHANG, I ;
FUJARA, F ;
GEIL, B ;
HEUBERGER, G ;
MANGEL, T ;
SILLESCU, H .
JOURNAL OF NON-CRYSTALLINE SOLIDS, 1994, 172 :248-255
[9]   A NEW TECHNIQUE FOR MEASURING ULTRASLOW MOLECULAR-REORIENTATION NEAR AND BELOW THE GLASS-TRANSITION [J].
CICERONE, MT ;
EDIGER, MD .
JOURNAL OF CHEMICAL PHYSICS, 1992, 97 (03) :2156-2159
[10]   PHOTOBLEACHING TECHNIQUE FOR MEASURING ULTRASLOW REORIENTATION NEAR AND BELOW THE GLASS-TRANSITION - TETRACENE IN O-TERPHENYL [J].
CICERONE, MT ;
EDIGER, MD .
JOURNAL OF PHYSICAL CHEMISTRY, 1993, 97 (40) :10489-10497