skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Dynamic cross-correlations between entangled biofilaments as they diffuse

Journal Article · · Proceedings of the National Academy of Sciences of the United States of America

Entanglement in polymer and biological physics involves a state in which linear interthreaded macromolecules in isotropic liquids diffuse in a spatially anisotropic manner beyond a characteristic mesoscopic time and length scale (tube diameter). The physical reason is that linear macromolecules become transiently localized in directions transverse to their backbone but diffuse with relative ease parallel to it. Within the resulting broad spectrum of relaxation times there is an extended period before the longest relaxation time when filaments occupy a time-averaged cylindrical space of near-constant density. Here we show its implication with experiments based on fluorescence tracking of dilutely labeled macromolecules. The entangled pairs of aqueous F-actin biofilaments diffuse with separation-dependent dynamic cross-correlations that exceed those expected from continuum hydrodynamics up to strikingly large spatial distances of ≈15 µm, which is more than 104 times the size of the solvent water molecules in which they are dissolved, and is more than 50 times the dynamic tube diameter, but is almost equal to the filament length. Modeling this entangled system as a collection of rigid rods, we present a statistical mechanical theory that predicts these long-range dynamic correlations as an emergent consequence of an effective long-range interpolymer repulsion due to the de Gennes correlation hole, which is a combined consequence of chain connectivity and uncrossability. The key physical assumption needed to make theory and experiment agree is that solutions of entangled biofilaments localized in tubes that are effectively dynamically incompressible over the relevant intermediate time and length scales.

Research Organization:
Univ. of Illinois at Urbana-Champaign, IL (United States); Ulsan National Inst. of Science and Technology (UNIST) (Korea, Republic of)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Inst. for Basic Science (IBS) (Korea, Republic of)
Grant/Contract Number:
FG02-07ER46471; FG02-02ER46019; IBS-R020-D1
OSTI ID:
1346579
Alternate ID(s):
OSTI ID: 1465692
Journal Information:
Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Vol. 114 Journal Issue: 13; ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 8 works
Citation information provided by
Web of Science

References (45)

Space-time correlated two-particle hopping in glassy fluids: Structural relaxation, irreversibility, decoupling, and facilitation journal June 2012
Many chain correlated dynamics in polymer fluids journal April 1999
Models for the Length Distributions of Actin Filaments: I. Simple Polymerization and Fragmentation journal May 1998
Brownian Motion of DNA Confined Within a Two-Dimensional Array journal August 2002
Macromolecular crowding: an important but neglected aspect of the intracellular environment journal February 2001
Connection between Polymer Molecular Weight, Density, Chain Dimensions, and Melt Viscoelastic Properties journal August 1994
Macromolecular Crowding and Confinement: Biochemical, Biophysical, and Potential Physiological Consequences journal June 2008
Two-Point Microrheology of Inhomogeneous Soft Materials journal July 2000
Local measurements of viscoelastic moduli of entangled actin networks using an oscillating magnetic bead micro-rheometer journal June 1994
Confining Potential when a Biopolymer Filament Reptates journal March 2010
Rheology and Microscopic Topology of Entangled Polymeric Liquids journal February 2004
Modeling semiflexible polymer networks journal July 2014
Fluid Mechanics of Microrheology journal January 2010
Localization of chain dynamics in entangled polymer melts journal May 2014
One- and two-point micro-rheology of viscoelastic media journal December 2002
Macromolecular crowding: obvious but underappreciated journal October 2001
The statistical mechanics of polymerized material journal September 1967
Anomalous yet Brownian journal July 2009
Supercooled liquids for pedestrians journal June 2009
Three-Dimensional Direct Imaging of Structural Relaxation Near the Colloidal Glass Transition journal January 2000
Microrheometry of semiflexible actin networks through enforced single-filament reptation: Frictional coupling and heterogeneities in entangled networks journal May 2002
Theory of correlated two-particle activated glassy dynamics: General formulation and heterogeneous structural relaxation in hard sphere fluids journal February 2011
Scattering of Slow Neutrons by a Liquid journal June 1958
Viscoelasticity of biopolymer networks and statistical mechanics of semiflexible polymers book January 1999
Methods to Track Single-Molecule Trajectories journal June 2006
Theory of dynamic critical phenomena journal July 1977
High-Frequency Stress Relaxation in Semiflexible Polymer Solutions and Networks journal April 2006
Pair diffusion at close range in liquids journal December 1986
Direct imaging of reptation for semiflexible actin filaments journal March 1994
Theory of nanoparticle diffusion in unentangled and entangled polymer melts journal December 2011
Molecular Theory of Brownian Motion for Several Particles journal April 1971
Force fluctuations and polymerization dynamics of intracellular microtubules journal October 2007
Rheology of Soft Materials journal August 2010
Direct Observation of the Dynamics of Semiflexible Polymers in Shear Flow journal March 2013
Diffusion of actin filaments within a thin layer between two walls journal June 2004
Liquid dynamics and inelastic scattering of neutrons journal January 1959
Screening of hydrodynamic interaction in a solution of rodlike macromolecules journal September 1983
Simulations of dynamics and viscoelasticity in highly entangled solutions of semiflexible rods journal July 2007
Screening of hydrodynamic interactions in Brownian rod suspensions journal April 2008
Spatially dependent relative diffusion of nanoparticles in polymer melts journal August 2013
Chain dynamics, mesh size, and diffusive transport in networks of polymerized actin: a quasielastic light scattering and microfluorescence study journal September 1989
Reptation of a Polymer Chain in the Presence of Fixed Obstacles journal July 1971
Tube diameter in tightly entangled solutions of semiflexible polymers journal February 2001
Universal Nature of Particle Displacements close to Glass and Jamming Transitions journal August 2007
Correlated two-particle diffusion in dense colloidal suspensions at early times: Theory and comparison to experiment journal November 2015

Similar Records

Theory of Nanoparticle Diffusion in Unentangled and Entangled Polymer Melts.
Journal Article · Sat Jan 01 00:00:00 EST 2011 · The Journal of Chemical Physics · OSTI ID:1346579

Segment-scale, force-level theory of mesoscopic dynamic localization and entropic elasticity in entangled chain polymer liquids
Journal Article · Tue Apr 04 00:00:00 EDT 2017 · Journal of Chemical Physics · OSTI ID:1346579

Nanorod Mobility within Entangled Wormlike Micelle Solutions
Journal Article · Tue Dec 20 00:00:00 EST 2016 · Macromolecules · OSTI ID:1346579