Self-diffusion of supercooled o-terphenyl near the glass transition temperature

被引:201
作者
Mapes, MK [1 ]
Swallen, SF [1 ]
Ediger, MD [1 ]
机构
[1] Univ Wisconsin, Dept Chem, Madison, WI 53706 USA
关键词
D O I
10.1021/jp0555955
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Self-diffusion coefficients for the low molecular weight glass former o-terphenyl have been measured near T-g by isothermally desorbing thin film bilayers of deuterio and protio o-terphenyl in a vacuum chamber. We observe translational diffusion that is about 100 times faster at T-g + 3 K than the Stokes-Einstein prediction. Predictions from random first order transition theory and a dynamic facilitation approach are in reasonable agreement with our results; in these approaches, enhanced translational diffusion is associated with spatially heterogeneous dynamics. Self-diffusion controls crystallization in o-terphenyl for most of the supercooled liquid regime, but at temperatures below T-g + 10 K, the reported crystallization rate increases suddenly while the self-diffusion coefficient does not. This work and previous work on trisnaphthylbenzene both find a self-diffusion-controlled crystal growth regime and an enhancement in self-diffusion near T-g, suggesting that these phenomena are general characteristics of fragile low molecular weight glass formers. We discuss the width of the relaxation time distributions of o-terphenyl and trisnaphthylbenzene as they relate to the observation of enhanced translational diffusion.
引用
收藏
页码:507 / 511
页数:5
相关论文
共 49 条
[1]   Length scale for the onset of Fickian diffusion in supercooled liquids [J].
Berthier, L ;
Chandler, D ;
Garrahan, JP .
EUROPHYSICS LETTERS, 2005, 69 (03) :320-326
[2]  
BOERJESSON L, 1990, CHEM PHYS, V149, P209
[3]   Heterogeneity at the glass transition: Translational and rotational self-diffusion [J].
Chang, I ;
Sillescu, H .
JOURNAL OF PHYSICAL CHEMISTRY B, 1997, 101 (43) :8794-8801
[4]   HOW DO MOLECULES MOVE NEAR T-G - MOLECULAR ROTATION OF 6 PROBES IN O-TERPHENYL ACROSS 14 DECADES IN TIME [J].
CICERONE, MT ;
BLACKBURN, FR ;
EDIGER, MD .
JOURNAL OF CHEMICAL PHYSICS, 1995, 102 (01) :471-479
[5]   RELAXATION OF SPATIALLY HETEROGENEOUS DYNAMIC DOMAINS IN SUPERCOOLED ORTHO-TERPHENYL [J].
CICERONE, MT ;
EDIGER, MD .
JOURNAL OF CHEMICAL PHYSICS, 1995, 103 (13) :5684-5692
[6]   Translational diffusion on heterogeneous lattices: A model for dynamics in glass forming materials [J].
Cicerone, MT ;
Wagner, PA ;
Ediger, MD .
JOURNAL OF PHYSICAL CHEMISTRY B, 1997, 101 (43) :8727-8734
[7]   RETRACTED: Single-molecule studies of heterogeneous dynamics in polymer melts near the class transition (Retracted article. See vol 312, pg 195, 2006) [J].
Deschenes, LA ;
Vanden Bout, DA .
SCIENCE, 2001, 292 (5515) :255-258
[8]   Rotational correlation functions and apparently enhanced translational diffusion in a free-energy landscape model for the α relaxation in glass-forming liquids [J].
Diezemann, G ;
Sillescu, H ;
Hinze, G ;
Bohmer, R .
PHYSICAL REVIEW E, 1998, 57 (04) :4398-4410
[9]   FREQUENCY-DEPENDENT SPECIFIC-HEAT AND THERMAL-CONDUCTIVITY AT THE GLASS-TRANSITION IN ORTHO-TERPHENYL MIXTURES [J].
DIXON, PK ;
NAGEL, SR .
PHYSICAL REVIEW LETTERS, 1988, 61 (03) :341-344
[10]   TRANSLATIONAL AND ROTATIONAL DIFFUSION IN SUPERCOOLED ORTHOTERPHENYL CLOSE TO THE GLASS-TRANSITION [J].
FUJARA, F ;
GEIL, B ;
SILLESCU, H ;
FLEISCHER, G .
ZEITSCHRIFT FUR PHYSIK B-CONDENSED MATTER, 1992, 88 (02) :195-204