Rouse mode analysis of chain relaxation in polymer nanocomposites

Kalathi, Jagannathan T.; Kumar, Sanat K.; Rubinstein, Michael; Grest, Gary S.

doi:10.1039/c5sm00754b

Title: Rouse mode analysis of chain relaxation in polymer nanocomposites

Journal Article · Mon Apr 20 00:00:00 EDT 2015 · Soft Matter

DOI:https://doi.org/10.1039/c5sm00754b· OSTI ID:1235359

Kalathi, Jagannathan T. ^[1]; Kumar, Sanat K. ^[2]; Rubinstein, Michael ^[3]; Grest, Gary S. ^[4]

Columbia Univ., New York, NY (United States). Dept. of Chemical Engineering; National Inst. of Technology Karnataka, Surathkal (India). Dept. of Chemical Engineering
Columbia Univ., New York, NY (United States). Dept. of Chemical Engineering
Univ. of North Carolina, Chapel Hill, NC (United States). Dept. of Chemistry
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Large-scale molecular dynamics simulations are used to study the internal relaxations of chains in nanoparticle (NP)/polymer composites. In this paper, we examine the Rouse modes of the chains, a quantity that is closest in spirit to the self-intermediate scattering function, typically determined in an (incoherent) inelastic neutron scattering experiment. Our simulations show that for weakly interacting mixtures of NPs and polymers, the effective monomeric relaxation rates are faster than in a neat melt when the NPs are smaller than the entanglement mesh size. In this case, the NPs serve to reduce both the monomeric friction and the entanglements in the polymer melt, as in the case of a polymer–solvent system. However, for NPs larger than half the entanglement mesh size, the effective monomer relaxation is essentially unaffected for low NP concentrations. Even in this case, we observe a strong reduction in chain entanglements for larger NP loadings. Furthermore, the role of NPs is to always reduce the number of entanglements, with this effect only becoming pronounced for small NPs or for high concentrations of large NPs. Finally, our studies of the relaxation of single chains resonate with recent neutron spin echo (NSE) experiments, which deduce a similar entanglement dilution effect.

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Research Organization:: Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Columbia Univ., New York, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE National Nuclear Security Administration (NNSA); National Science Foundation (NSF); National Inst. of Health (NIH) (United States); Cystic Fibrosis Foundation (United States)

Contributing Organization:: Univ. of North Carolina, Chapel Hill, NC (United States); National Inst. of Technology Karnataka, Surathkal (India)

Grant/Contract Number:: AC04-94AL85000; AC02-05CH11231; DMR-1006514; DMR-1309892; DMR-1436201; DMR-1121107; DMR-1122483; 1-P01-HL108808-01A1

OSTI ID:: 1235359

Alternate ID(s):: OSTI ID: 1340251

Report Number(s):: SAND-2015-2617J; SAND2014-19679J; SMOABF; 581967

Journal Information:: Soft Matter, Vol. 11, Issue 20; ISSN 1744-683X

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 61 works

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