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Transport dynamics of complex fluids.
Song, Sanggeun; Park, Seong Jun; Kim, Minjung; Kim, Jun Soo; Sung, Bong June; Lee, Sangyoub; Kim, Ji-Hyun; Sung, Jaeyoung.
  • Song S; Creative Research Initiative Center for Chemical Dynamics in Living Cells, Chung-Ang University, 06974 Seoul, Republic of Korea.
  • Park SJ; Department of Chemistry, Chung-Ang University, 06974 Seoul, Republic of Korea.
  • Kim M; National Institute of Innovative Functional Imaging, Chung-Ang University, 06974 Seoul, Republic of Korea.
  • Kim JS; Creative Research Initiative Center for Chemical Dynamics in Living Cells, Chung-Ang University, 06974 Seoul, Republic of Korea.
  • Sung BJ; Department of Chemistry, Chung-Ang University, 06974 Seoul, Republic of Korea.
  • Lee S; National Institute of Innovative Functional Imaging, Chung-Ang University, 06974 Seoul, Republic of Korea.
  • Kim JH; Department of Chemistry, College of Natural Sciences, Seoul National University, 08826 Seoul, Republic of Korea.
  • Sung J; Department of Chemistry and Nanoscience, Ewha Womans University, 03760 Seoul, Republic of Korea.
Proc Natl Acad Sci U S A ; 116(26): 12733-12742, 2019 06 25.
Article en En | MEDLINE | ID: mdl-31175151
Thermal motion in complex fluids is a complicated stochastic process but ubiquitously exhibits initial ballistic, intermediate subdiffusive, and long-time diffusive motion, unless interrupted. Despite its relevance to numerous dynamical processes of interest in modern science, a unified, quantitative understanding of thermal motion in complex fluids remains a challenging problem. Here, we present a transport equation and its solutions, which yield a unified quantitative explanation of the mean-square displacement (MSD), the non-Gaussian parameter (NGP), and the displacement distribution of complex fluids. In our approach, the environment-coupled diffusion kernel and its time correlation function (TCF) are the essential quantities that determine transport dynamics and characterize mobility fluctuation of complex fluids; their time profiles are directly extractable from a model-free analysis of the MSD and NGP or, with greater computational expense, from the two-point and four-point velocity autocorrelation functions. We construct a general, explicit model of the diffusion kernel, comprising one unbound-mode and multiple bound-mode components, which provides an excellent approximate description of transport dynamics of various complex fluidic systems such as supercooled water, colloidal beads diffusing on lipid tubes, and dense hard disk fluid. We also introduce the concepts of intrinsic disorder and extrinsic disorder that have distinct effects on transport dynamics and different dependencies on temperature and density. This work presents an unexplored direction for quantitative understanding of transport and transport-coupled processes in complex disordered media.
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