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Title: Untangleing the effects of chain rigidity on the structure and dynamics of strongly adsorbed polymer melts

Abstract

Here, we present a detailed analysis of coarse-grained molecular dynamics simulations of semiflexible polymer melts in contact with a strongly adsorbing substrate. We have characterized the segments in the interfacial layer by counting the number of trains, loops, tails and unadsorbed segments. For more rigid chains, a tail and an adsorbed segment (a train) dominate while loops are more prevalent in more flexible chains. The tails exhibit a non-uniformly stretched conformation akin to the polydispersed pseudobrush envisioned by Guiselin. To probe the dynamics of the segments we computed the layer z-resolved intermediate coherent collective dynamics structure factor, S(q, t, z), mean-square displacement of segments, and the 2nd Legendre polynomial of the time-autocorrelation of unit bond vectors, 2[ni(t,z)•ni(0,z)]>. Our results show that segmental dynamics is slower for stiffer chains and there is a strong correlation between the structure and dynamics in the interfacial layer. There is no glassy layer, and the slowing down in dynamics of stiffer chains in the adsorbed region can be attributed to the densification and the more persistent layering of segments.

Authors:
 [1];  [1];  [1];  [1];  [2];  [1]
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  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1190760
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Macromolecules
Additional Journal Information:
Journal Volume: 48; Journal Issue: 12; Journal ID: ISSN 0024-9297
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Carrillo, Jan-Michael Y., Cheng, Shiwang, Kumar, Rajeev, Goswami, Monojoy, Sokolov, Alexei P, and Sumpter, Bobby G. Untangleing the effects of chain rigidity on the structure and dynamics of strongly adsorbed polymer melts. United States: N. p., 2015. Web. doi:10.1021/acs.macromol.5b00624.
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Carrillo, Jan-Michael Y., Cheng, Shiwang, Kumar, Rajeev, Goswami, Monojoy, Sokolov, Alexei P, & Sumpter, Bobby G. Untangleing the effects of chain rigidity on the structure and dynamics of strongly adsorbed polymer melts. United States. https://doi.org/10.1021/acs.macromol.5b00624
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Carrillo, Jan-Michael Y., Cheng, Shiwang, Kumar, Rajeev, Goswami, Monojoy, Sokolov, Alexei P, and Sumpter, Bobby G. Thu . "Untangleing the effects of chain rigidity on the structure and dynamics of strongly adsorbed polymer melts". United States. https://doi.org/10.1021/acs.macromol.5b00624. https://www.osti.gov/servlets/purl/1190760.
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@article{osti_1190760,
title = {Untangleing the effects of chain rigidity on the structure and dynamics of strongly adsorbed polymer melts},
author = {Carrillo, Jan-Michael Y. and Cheng, Shiwang and Kumar, Rajeev and Goswami, Monojoy and Sokolov, Alexei P and Sumpter, Bobby G.},
abstractNote = {Here, we present a detailed analysis of coarse-grained molecular dynamics simulations of semiflexible polymer melts in contact with a strongly adsorbing substrate. We have characterized the segments in the interfacial layer by counting the number of trains, loops, tails and unadsorbed segments. For more rigid chains, a tail and an adsorbed segment (a train) dominate while loops are more prevalent in more flexible chains. The tails exhibit a non-uniformly stretched conformation akin to the polydispersed pseudobrush envisioned by Guiselin. To probe the dynamics of the segments we computed the layer z-resolved intermediate coherent collective dynamics structure factor, S(q, t, z), mean-square displacement of segments, and the 2nd Legendre polynomial of the time-autocorrelation of unit bond vectors, 2[ni(t,z)•ni(0,z)]>. Our results show that segmental dynamics is slower for stiffer chains and there is a strong correlation between the structure and dynamics in the interfacial layer. There is no glassy layer, and the slowing down in dynamics of stiffer chains in the adsorbed region can be attributed to the densification and the more persistent layering of segments.},
doi = {10.1021/acs.macromol.5b00624},
journal = {Macromolecules},
number = 12,
volume = 48,
place = {United States},
year = {Thu Jun 11 00:00:00 EDT 2015},
month = {Thu Jun 11 00:00:00 EDT 2015}
}
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https://doi.org/10.1021/acs.macromol.5b00624
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