Ideal probe single-molecule experiments reveal the intrinsic dynamic heterogeneity of a supercooled liquid

被引:62
作者
Paeng, Keewook [1 ,2 ]
Park, Heungman [1 ]
Hoang, Dat Tien [1 ]
Kaufman, Laura J. [1 ]
机构
[1] Columbia Univ, Dept Chem, New York, NY 10027 USA
[2] Sungkyunkwan Univ, Dept Chem, Suwon 440746, South Korea
基金
美国国家科学基金会;
关键词
supercooled liquid; dynamic heterogeneity; single molecule; ergodicity; fluorescence; GLASS-TRANSITION; O-TERPHENYL; T-G; DYE MOLECULES; LENGTH SCALE; REORIENTATION; FLUORESCENCE; RELAXATION; GLYCEROL; ROTATION;
D O I
10.1073/pnas.1424636112
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
The concept of dynamic heterogeneity and the picture of the supercooled liquid as a mosaic of environments with distinct dynamics that interchange in time have been invoked to explain the nonexponential relaxations measured in these systems. The spatial extent and temporal persistence of these regions of distinct dynamics have remained challenging to identify. Here, single-molecule fluorescence measurements using a probe similar in size and mobility to the host o-terphenyl unambiguously reveal exponential relaxations distributed in time and space and directly demonstrate ergodicity of the system down to the glass transition temperature. In the temperature range probed, at least 200 times the structural relaxation time of the host is required to recover ensemble-averaged relaxation at every spatial region in the system.
引用
收藏
页码:4952 / 4957
页数:6
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