Title: Correlated two-particle diffusion in dense colloidal suspensions at early times: Theory and comparison to experiment

Journal Article · · Physical Review. E, Statistical, Nonlinear, and Soft Matter Physics
 [1];  [2];  [2];  [3];  [2]
  1. Univ. of Illinois at Urbana-Champaign, IL (United States); University of Illinois
  2. Univ. of Illinois at Urbana-Champaign, IL (United States)
  3. Univ. of Illinois at Urbana-Champaign, IL (United States); Inst. of Basic Science, Daejeon (Korea, Republic of); Ulsan National Institute of Science and Technology (UNIST), Ulsan (Korea, Republic of)
+ Show Author Affiliations

The spatially resolved diffusive dynamic cross correlations of a pair of colloids in dense quasi-two-dimensional monolayers of identical particles are studied experimentally and theoretically at early times where motion is Fickian. In very dense systems where strong oscillatory equilibrium packing correlations are present, we find an exponential decay of the dynamic cross correlations on small and intermediate length scales. At large separations where structure becomes random, an apparent power law decay with an exponent of approximately –2.2 is observed. For a moderately dense suspension where local structural correlations are essentially absent, this same apparent power law decay is observed over all probed interparticle separations. A microscopic nonhydrodynamic theory is constructed for the dynamic cross correlations which is based on interparticle frictional effects and effective structural forces. Hydrodynamics enters only via setting the very short-time single-particle self-diffusion constant. No-adjustable-parameter quantitative predictions of the theory for the dynamic cross correlations are in good agreement with experiment over all length scales. The origin of the long-range apparent power law is the influence of the constraint of fixed interparticle separation on the amplitude of the mean square force exerted on the two tagged particles by the surrounding fluid. The theory is extended to study high-packing-fraction 3D hard sphere fluids. Here, the same pattern of an oscillatory exponential form of the dynamic cross correlation function is predicted in the structural regime, but the long-range tail decays faster than in monolayers with an exponent of –3.

Research Organization:
Univ. of Illinois at Urbana-Champaign, IL (United States)
Sponsoring Organization:
USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
FG02-07ER46471
OSTI ID:
1875117
Journal Information:
Physical Review. E, Statistical, Nonlinear, and Soft Matter Physics, Journal Name: Physical Review. E, Statistical, Nonlinear, and Soft Matter Physics Journal Issue: 5 Vol. 92; ISSN 1539-3755
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

References (36)

On Edge-Corrected Kernel-Based Pair-Correlation Function Estimators for Point Processes journal January 1990
Liquid dynamics and inelastic scattering of neutrons journal January 1959
Diffusion of spheres in a concentrated suspension: Resummation of many-body hydrodynamic interactions journal October 1983
Diffusion of spheres in a concentrated suspension II journal July 1984
Topological character of hydrodynamic screening in suspensions of hard spheres: An example of universal phenomenon journal August 2009
Instantaneous Normal Modes and Cooperative Dynamics in a Quasi-Two-Dimensional System of Particles journal April 2004
Screening of hydrodynamic interaction in a solution of rodlike macromolecules journal September 1983
Molecular Theory of Brownian Motion for Several Particles journal April 1971
Screening of hydrodynamic interactions in Brownian rod suspensions journal April 2008
Theory of correlated two-particle activated glassy dynamics: General formulation and heterogeneous structural relaxation in hard sphere fluids journal February 2011
On the Stokes problem for a suspension of spheres at finite concentrations journal March 1978
Pair diffusion at close range in liquids journal December 1986
Microscopic theory of the dynamics of polymeric liquids: General formulation of a mode–mode‐coupling approach journal November 1989
An accurate and simple equation of state for hard disks journal September 1995
Many chain correlated dynamics in polymer fluids journal April 1999
Spatially dependent relative diffusion of nanoparticles in polymer melts journal August 2013
Dynamic simulation of concentrated macromolecular solutions with screened long-range hydrodynamic interactions: Algorithm and limitations journal September 2013
Analysis of the Brinkman equation as a model for flow in porous media journal January 1987
XXVII. A brief account of microscopical observations made in the months of June, July and August 1827, on the particles contained in the pollen of plants; and on the general existence of active molecules in organic and inorganic bodies journal September 1828
Relaxation processes in supercooled liquids journal March 1992
Physics in ordered and disordered colloidal matter composed of poly( N -isopropylacrylamide) microgel particles journal May 2014
One- and two-point micro-rheology of viscoelastic media journal December 2002
Correlated particle dynamics in concentrated quasi-two-dimensional suspensions journal November 2005
Scattering of Slow Neutrons by a Liquid journal June 1958
Connections between some kinetic and equilibrium theories of the glass transition journal April 1987
Experimental observations of non-Gaussian behavior and stringlike cooperative dynamics in concentrated quasi-two-dimensional colloidal liquids journal November 1999
Two-point microrheology and the electrostatic analogy journal December 2001
Theory of coupled translational-rotational glassy dynamics in dense fluids of uniaxial particles journal July 2009
Space-time correlated two-particle hopping in glassy fluids: Structural relaxation, irreversibility, decoupling, and facilitation journal June 2012
Structural responses of quasi-two-dimensional colloidal fluids to excitations elicited by nonequilibrium perturbations journal September 2012
Divergence of the long-wavelength collective diffusion coefficient in quasi-one- and quasi-two-dimensional colloidal suspensions journal February 2014
Hydrodynamic Coupling of Two Brownian Spheres to a Planar Surface journal October 2000
Effective Screening of Hydrodynamic Interactions in Charged Colloidal Suspensions journal December 2000
Two-Point Microrheology of Inhomogeneous Soft Materials journal July 2000
Fluid Mechanics of Microrheology journal January 2010
Correlated Diffusion of Colloidal Particles near a Liquid-Liquid Interface journal January 2014

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72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS