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

Carrillo, Jan-Michael Y.; Cheng, Shiwang; Kumar, Rajeev; Goswami, Monojoy; Sokolov, Alexei P; Sumpter, Bobby G.

doi:10.1021/acs.macromol.5b00624

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

Journal Article · Thu Jun 11 00:00:00 EDT 2015 · Macromolecules

DOI:https://doi.org/10.1021/acs.macromol.5b00624· OSTI ID:1190760

Carrillo, Jan-Michael Y. ^[1]; Cheng, Shiwang ^[1]; Kumar, Rajeev ^[1]; Goswami, Monojoy ^[1]; Sokolov, Alexei P ^[2]; Sumpter, Bobby G. ^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)

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[n_i(t,z)•n_i(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.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1190760

Journal Information:: Macromolecules, Vol. 48, Issue 12; ISSN 0024-9297

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 92 works

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