Ideal probe single-molecule experiments reveal the intrinsic dynamic heterogeneity of a supercooled liquid
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作者:
Paeng, Keewook
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Columbia Univ, Dept Chem, New York, NY 10027 USA
Sungkyunkwan Univ, Dept Chem, Suwon 440746, South KoreaColumbia Univ, Dept Chem, New York, NY 10027 USA
Paeng, Keewook
[1
,2
]
Park, Heungman
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Columbia Univ, Dept Chem, New York, NY 10027 USAColumbia Univ, Dept Chem, New York, NY 10027 USA
Park, Heungman
[1
]
Hoang, Dat Tien
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Columbia Univ, Dept Chem, New York, NY 10027 USAColumbia Univ, Dept Chem, New York, NY 10027 USA
Hoang, Dat Tien
[1
]
Kaufman, Laura J.
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Columbia Univ, Dept Chem, New York, NY 10027 USAColumbia Univ, Dept Chem, New York, NY 10027 USA
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
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.
机构:
CNRS, UMR 5221, Lab Charles Coulomb, Montpellier, France
Univ Montpellier 2, Montpellier, FranceCNRS, UMR 5221, Lab Charles Coulomb, Montpellier, France
Berthier, Ludovic
Biroli, Giulio
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机构:
CEA, IPhT, Inst Phys Theor, F-91191 Gif Sur Yvette, France
CNRS, URA 2306, F-75700 Paris, FranceCNRS, UMR 5221, Lab Charles Coulomb, Montpellier, France
机构:
CNRS, UMR 5221, Lab Charles Coulomb, Montpellier, France
Univ Montpellier 2, Montpellier, FranceCNRS, UMR 5221, Lab Charles Coulomb, Montpellier, France
Berthier, Ludovic
Biroli, Giulio
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h-index: 0
机构:
CEA, IPhT, Inst Phys Theor, F-91191 Gif Sur Yvette, France
CNRS, URA 2306, F-75700 Paris, FranceCNRS, UMR 5221, Lab Charles Coulomb, Montpellier, France