Single-molecule studies of heterogeneous dynamics in polymer melts near the glass transition.
作者： Laura A Deschenes , David A Vanden Bout
关键词: Single probe 、 Nuclear magnetic resonance 、 Molecule 、 Spectroscopy 、 Local environment 、 Chemical physics 、 Scale (ratio) 、 Polymer 、 Glass transition 、 Chemistry 、 Dynamics (mechanics)
摘要: Single-molecule spectroscopy was used to follow the orientation of a single probe molecule in polymer film real time. Broad spatially heterogeneous dynamics were observed on long time scales, which result from simple diffusive rotational motions short scales. This behavior persists for many rotations before molecule's local environment changes one characterized by new scale. environmental exchange occurs instantaneously scale experiment and may arise large-scale collective motions. The distribution times these environments measured several temperatures near glass transition.
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Christoph Bennemann, Claudio Donati, Jörg Baschnagel, Sharon C. Glotzer, Growing range of correlated motion in a polymer melt on cooling towards the glass transition Nature. ,vol. 399, pp. 246- 249 ,(1999) , 10.1038/20406
Robert M. Dickson, Andrew B. Cubitt, Roger Y. Tsien, W. E. Moerner, On/off blinking and switching behaviour of single molecules of green fluorescent protein Nature. ,vol. 388, pp. 355- 358 ,(1997) , 10.1038/41048
E. Vidal Russell, N. E. Israeloff, Direct observation of molecular cooperativity near the glass transition Nature. ,vol. 408, pp. 695- 698 ,(2000) , 10.1038/35047037
Gerold Adam, Julian H. Gibbs, On the Temperature Dependence of Cooperative Relaxation Properties in Glass‐Forming Liquids Journal of Chemical Physics. ,vol. 43, pp. 139- 146 ,(1965) , 10.1063/1.1696442
Eric R Weeks, John C Crocker, Andrew C Levitt, Andrew Schofield, David A Weitz, Three-Dimensional Direct Imaging of Structural Relaxation Near the Colloidal Glass Transition Science. ,vol. 287, pp. 627- 631 ,(2000) , 10.1126/SCIENCE.287.5453.627
Tobias Gleim, Walter Kob, Kurt Binder, How Does the Relaxation of a Supercooled Liquid Depend on Its Microscopic Dynamics Physical Review Letters. ,vol. 81, pp. 4404- 4407 ,(1998) , 10.1103/PHYSREVLETT.81.4404
C. A. Angell, K. L. Ngai, G. B. McKenna, P. F. McMillan, S. W. Martin, Relaxation in glassforming liquids and amorphous solids Journal of Applied Physics. ,vol. 88, pp. 3113- 3157 ,(2000) , 10.1063/1.1286035
S Nie, D. Chiu, R. Zare, Probing individual molecules with confocal fluorescence microscopy Science. ,vol. 266, pp. 1018- 1021 ,(1994) , 10.1126/SCIENCE.7973650
W. E. Moerner, Examining Nanoenvironments in Solids on the Scale of a Single, Isolated Impurity Molecule Science. ,vol. 265, pp. 46- 53 ,(1994) , 10.1126/SCIENCE.265.5168.46
Hans Sillescu, Heterogeneity at the glass transition: a review Journal of Non-crystalline Solids. ,vol. 243, pp. 81- 108 ,(1999) , 10.1016/S0022-3093(98)00831-X