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Title: Nanorheology of Entangled Polymer Melts

Abstract

In this study, we use molecular simulations to probe the local viscoelasticity of an entangled polymer melt by tracking the motion of embedded nonsticky nanoparticles (NPs). As in conventional microrheology, the generalized Stokes-Einstein relation is employed to extract an effective stress relaxation function GGSE(t) from the mean square displacement of NPs. GGSE(t) for different NP diameters d are compared with the stress relaxation function G(t) of a pure polymer melt. The deviation of GGSE(t) from G(t) reflects the incomplete coupling between NPs and the dynamic modes of the melt. For linear polymers, a plateau in GGSE(t) emerges as d exceeds the entanglement mesh size a and approaches the entanglement plateau in G(t) for a pure melt with increasing d. For ring polymers, as d increases towards the spanning size R of ring polymers, GGSE(t) approaches G(t) of the ring melt with no entanglement plateau.

Authors:
 [1];  [2];  [1]
+ Show Author Affiliations
  1. Univ. of North Carolina, Chapel Hill, NC (United States). Department of Chemistry
  2. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Publication Date:
Research Org.:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC)
OSTI Identifier:
1430900
Alternate Identifier(s):
OSTI ID: 1419116
Report Number(s):
SAND-2018-0707J
Journal ID: ISSN 0031-9007; PRLTAO; 660141; TRN: US1802636
Grant/Contract Number:  
AC04-94AL85000; AC02-05CH11231; NA0003525
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 120; Journal Issue: 5; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Ge, Ting, Grest, Gary S., and Rubinstein, Michael. Nanorheology of Entangled Polymer Melts. United States: N. p., 2018. Web. https://doi.org/10.1103/PhysRevLett.120.057801.
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Ge, Ting, Grest, Gary S., & Rubinstein, Michael. Nanorheology of Entangled Polymer Melts. United States. https://doi.org/10.1103/PhysRevLett.120.057801
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Ge, Ting, Grest, Gary S., and Rubinstein, Michael. Thu . "Nanorheology of Entangled Polymer Melts". United States. https://doi.org/10.1103/PhysRevLett.120.057801. https://www.osti.gov/servlets/purl/1430900.
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@article{osti_1430900,
title = {Nanorheology of Entangled Polymer Melts},
author = {Ge, Ting and Grest, Gary S. and Rubinstein, Michael},
abstractNote = {In this study, we use molecular simulations to probe the local viscoelasticity of an entangled polymer melt by tracking the motion of embedded nonsticky nanoparticles (NPs). As in conventional microrheology, the generalized Stokes-Einstein relation is employed to extract an effective stress relaxation function GGSE(t) from the mean square displacement of NPs. GGSE(t) for different NP diameters d are compared with the stress relaxation function G(t) of a pure polymer melt. The deviation of GGSE(t) from G(t) reflects the incomplete coupling between NPs and the dynamic modes of the melt. For linear polymers, a plateau in GGSE(t) emerges as d exceeds the entanglement mesh size a and approaches the entanglement plateau in G(t) for a pure melt with increasing d. For ring polymers, as d increases towards the spanning size R of ring polymers, GGSE(t) approaches G(t) of the ring melt with no entanglement plateau.},
doi = {10.1103/PhysRevLett.120.057801},
journal = {Physical Review Letters},
number = 5,
volume = 120,
place = {United States},
year = {2018},
month = {2}
}
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Journal Article:
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https://doi.org/10.1103/PhysRevLett.120.057801
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Cited by: 2 works
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Figures / Tables:

FIG. 1 FIG. 1: GGSE(t) (open squares) for d = 5σ in linear polymers with N = 800. The corresponding 〈 ∆r2(t) 〉 is shown in the inset (see black line). The log-log slope α = 2 for the ballistic regime and α = 1 for the Fickian regime are indicated. Themore » estimated end of the crossover between ballistic and thermal motion is indicated by the black square.« less
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    Works referencing / citing this record:

    Investigation of the properties of nanographene in polymer nanocomposites through molecular simulations: dynamics and anisotropic Brownian motion
    journal, January 2019

    • Rissanou, Anastassia N.; Bačová, Petra; Harmandaris, Vagelis
    • Physical Chemistry Chemical Physics, Vol. 21, Issue 43
    • DOI: 10.1039/c9cp02074h

    A practical method to account for random phase approximation effects on the dynamic scattering of multi-component polymer systems
    journal, February 2020

    • Monkenbusch, M.; Kruteva, M.; Zamponi, M.
    • The Journal of Chemical Physics, Vol. 152, Issue 5
    • DOI: 10.1063/1.5139712

    Optical Tweezers Microrheology Maps the Dynamics of Strain-Induced Local Inhomogeneities in Entangled Polymers
    journal, July 2019

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