Literature DB >> 25825739

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

Keewook Paeng1, Heungman Park2, Dat Tien Hoang2, Laura J Kaufman3.   

Abstract

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.

Keywords:  dynamic heterogeneity; ergodicity; fluorescence; single molecule; supercooled liquid

Year:  2015        PMID: 25825739      PMCID: PMC4413315          DOI: 10.1073/pnas.1424636112

Source DB:  PubMed          Journal:  Proc Natl Acad Sci U S A        ISSN: 0027-8424            Impact factor:   11.205


  17 in total

1.  Spatially heterogeneous dynamics in supercooled liquids.

Authors:  M D Ediger
Journal:  Annu Rev Phys Chem       Date:  2000       Impact factor: 12.703

2.  Probe dependence of spatially heterogeneous dynamics in supercooled glycerol as revealed by single molecule microscopy.

Authors:  Stephan A Mackowiak; Lindsay M Leone; Laura J Kaufman
Journal:  Phys Chem Chem Phys       Date:  2010-11-26       Impact factor: 3.676

3.  Temperature dependent single molecule rotational dynamics in PMA.

Authors:  Subhasis Adhikari; Markus Selmke; Frank Cichos
Journal:  Phys Chem Chem Phys       Date:  2010-12-23       Impact factor: 3.676

4.  On the dielectric susceptibility spectra of supercooled o-terphenyl.

Authors:  Ranko Richert
Journal:  J Chem Phys       Date:  2005-10-15       Impact factor: 3.488

5.  Local viscosity of supercooled glycerol near Tg probed by rotational diffusion of ensembles and single dye molecules.

Authors:  Rob Zondervan; Florian Kulzer; Gregorius C G Berkhout; Michel Orrit
Journal:  Proc Natl Acad Sci U S A       Date:  2007-05-08       Impact factor: 11.205

6.  Single molecule rotational probing of supercooled liquids.

Authors:  Keewook Paeng; Laura J Kaufman
Journal:  Chem Soc Rev       Date:  2014-02-21       Impact factor: 54.564

7.  Single molecule probe reports of dynamic heterogeneity in supercooled ortho-terphenyl.

Authors:  Lindsay M Leone; Laura J Kaufman
Journal:  J Chem Phys       Date:  2013-03-28       Impact factor: 3.488

8.  Extraction of rotational correlation times from noisy single molecule fluorescence trajectories.

Authors:  Dat Tien Hoang; Keewook Paeng; Heungman Park; Lindsay M Leone; Laura J Kaufman
Journal:  Anal Chem       Date:  2014-09-03       Impact factor: 6.986

9.  Dynamic coupling of a small rigid probe to viscous ortho-terphenyl.

Authors:  Wei Huang; Ranko Richert
Journal:  J Chem Phys       Date:  2010-12-07       Impact factor: 3.488

10.  Nonexponential relaxation of poly(cyclohexyl acrylate): comparison of single-molecule and ensemble fluorescence studies.

Authors:  Chia-Yin Joyce Wei; David A Vanden Bout
Journal:  J Phys Chem B       Date:  2009-02-26       Impact factor: 2.991

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  6 in total

1.  Probing liquid dynamics, one molecule at a time.

Authors:  Ranko Richert
Journal:  Proc Natl Acad Sci U S A       Date:  2015-04-06       Impact factor: 11.205

2.  Correlated matrix-fluctuation-mediated activated transport of dilute penetrants in glass-forming liquids and suspensions.

Authors:  Rui Zhang; Kenneth S Schweizer
Journal:  J Chem Phys       Date:  2017-05-21       Impact factor: 3.488

3.  Viscosity of deeply supercooled water and its coupling to molecular diffusion.

Authors:  Amine Dehaoui; Bruno Issenmann; Frédéric Caupin
Journal:  Proc Natl Acad Sci U S A       Date:  2015-09-16       Impact factor: 11.205

4.  Fluid Phase Coexistence in Biological Membrane: Insights from Local Nonaffine Deformation of Lipids.

Authors:  Sahithya S Iyer; Madhusmita Tripathy; Anand Srivastava
Journal:  Biophys J       Date:  2018-07-03       Impact factor: 4.033

5.  Elucidation of the physical factors that control activated transport of penetrants in chemically complex glass-forming liquids.

Authors:  Baicheng Mei; Grant S Sheridan; Christopher M Evans; Kenneth S Schweizer
Journal:  Proc Natl Acad Sci U S A       Date:  2022-10-04       Impact factor: 12.779

6.  Single molecule demonstration of Debye-Stokes-Einstein breakdown in polystyrene near the glass transition temperature.

Authors:  Nicole L Mandel; Soohyun Lee; Kimyung Kim; Keewook Paeng; Laura J Kaufman
Journal:  Nat Commun       Date:  2022-06-23       Impact factor: 17.694

  6 in total

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