Long-Range Effects on Polymer Diffusion Induced by a Bounding Interface

Zheng, Xuemei; Rafailovich, Miriam; Sokolov, Jonathan; Strzhemechny, Yuri M.; Schwarz, S. A.; Sauer, Bryan B.; Rubinstein, Michael

doi:10.1103/physrevlett.79.241

Cited by 284 publications

(349 citation statements)

References 28 publications

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“…Consequently, the large spin-coating-induced deformation of the chains cannot relax. The strained interfacial sublayer can be pictured as highly disentangled and laterally anisotropic, with a thickness on the order of R g (43). The polymers adjacent to the surface immobilized sublayer can diffuse through the sublayer's pores forming a two-fluidsystem, as observed in diffusion measurements in a PS system (40).…”

Section: A)mentioning

confidence: 81%

“…The polymers adjacent to the surface immobilized sublayer can diffuse through the sublayer's pores forming a two-fluidsystem, as observed in diffusion measurements in a PS system (40). At a distance of about 7 to 10 R g apart from the substrate, the polymer behaves like the bulk elastomer and loses any memory of the presence of the silicon surface and the spin-coated induced interfacial alignment (40,43). We observe this transition from an induced interfacial alignment to the bulk elastomer as t c .…”

Section: A)mentioning

confidence: 86%

“…Existing classical mean field or molecular dynamic theories assume that the surface interaction is completely screened within a distance corresponding to the persistence length of the polymer (about 0.6 nm) (41,42). It was, however, found that this assumption is not valid in the case of spin-coated films where a layer immediately adjacent to the silicon substrate is pinned to the surface (40,43). Consequently, the large spin-coating-induced deformation of the chains cannot relax.…”

Section: A)mentioning

confidence: 97%

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Glass Transition Measurements of Ultrathin Polystyrene Films

Buenviaje

Dinelli

Overney

2000

ACS Symposium Series

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Data from various experiments suggest that the mechanical properties of thin polymer films depend, in a complex manner, on the film preparation process, in conjunction with interfacial interactions. In this paper, we discuss how and why interfacial interactions can affect the shear mechanical properties of spincoated polymer films. For example, confinement effects due to the spin coating process have been observed to exceed the nearest neighbor interaction distances by one order of magnitude. We introduce shear modulation scanning probe microscopy (SPM) as a technique to measure local shear property changes in thin polymer films as a function of temperature. Comparisons with bulk and lateral force measurements demonstrate the reliability of the technique. Using the shear modulation SPM, we observe a molecular weight dependence on the bulk glass transition. Measurements taken on polystyrene surfaces of various film thickness provide insight into how the glass transition of films are affected by substrate confinement.2

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Section: A)mentioning

confidence: 81%

Section: A)mentioning

confidence: 86%

Section: A)mentioning

confidence: 97%

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Glass Transition Measurements of Ultrathin Polystyrene Films

Buenviaje

Dinelli

Overney

2000

ACS Symposium Series

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“…This question belongs to the area of polymer-interface problems (Fleer et al 1993;Jones et al 1999). Although there is a large amount of both experimental (Zheng et al 1997;Frank et al 1996;Lin et al 1997;Rivilon et al 2000;Anastasiadis et al 2000;Fotiadou et al 2010;Chrissopoulou et al 2011) and simulation studies (Mansfield et al 1989 and1991;Bitsanis et al 1990;Rissanou et al 2009;Karaiskos et al 2009) on the general topic of polymer/solid interfaces, here we focus more on polymer/graphene (or polymer/graphite) simulation works, which are more relevant to our work. In more detail, Harmandaris et al and Daoulas et al (Daoulas et al 2005), in a series of two papers reported on modeling of hybrid polymer/graphite systems, through state-of-the-art atomistic Monte Carlo and Molecular Dynamics (MD) simulations.…”

Section: Introductionmentioning

confidence: 99%

Structure and dynamics of poly(methyl methacrylate)/graphene systems through atomistic molecular dynamics simulations

Rissanou

Harmandaris

2013

J Nanopart Res

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The main goal of the present work is to examine the effect of graphene layers on the structural and dynamical properties of polymer systems. We study hybrid poly(methyl methacrylate) (PMMA)/graphene interfacial systems, through detailed atomistic molecular dynamics (MD) simulations. In order to characterize the interface, various properties related to density, structure and dynamics of polymer chains are calculated, as a function of the distance from the substrate. A series of different hybrid systems, with width ranging between [2. 60 -13.35] nm, are being modeled. In addition, we compare the properties of the macromolecular chains to the properties of the corresponding bulk system at the same temperature. We observe a strong effect of graphene layers on both structure and dynamics of the PMMA chains. Furthermore the PMMA/graphene interface is characterized by different length scales, depending on the actual property we probe:Density of PMMA polymer chains is larger than the bulk value, for polymer chains close

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“…This would be so not just because of altered chain conformations, which would present additional points of contact with the surface compared with the case of a random coil, but also because motion might then be rate-limited by Arrhenius adsorption-desorption events rather than by intersegmental monomeric friction. There is copious evidence from experiment 3,4 and many computer simulations of the qualitative effect.…”

Section: Introductionmentioning

confidence: 99%

Surface Diffusion of Poly(ethylene glycol)

et al. 2002

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We report direct measurement of the center-of-mass diffusion coefficient, D, of uncharged flexible linear chains adsorbed at the solid-liquid interface at dilute surface coverage. We find D ∼ N -3/2 (N is degree of polymerization) when N was varied by more than an order of magnitude (N ) 48, 113, 244, 456, and 693) and the scatter of the data was low. The experimental system was poly(ethylene glycol), PEG, adsorbed from dilute aqueous solution onto a self-assembled hydrophobic monolayer, condensed octadecyltriethoxysilane. The method of measurement was fluorescence correlation spectroscopy of a rhodamine green derivative dye that was end-attached to one sole end of the adsorbed PEG chains. The observed scaling implies the diffusion time τ ∼ N 3 if Rg ∼ N 3/4 as expected for a chain in good solvent in two dimensions (Rg is the radius of gyration), but a variety of other theoretical approaches to describe the dynamical scaling are also plausible. The multiplicity of plausible dynamical transport scenarios is compounded by the fact that polymer diffusion is sensitive to chain conformation on the surface which is not directly observable. Various theoretical scenarios are explored, and the need for new experiments, theory, and computer simulation studies to allow definitive interpretation of this observation of simple and clean fractional power law scaling is emphasized.

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Long-Range Effects on Polymer Diffusion Induced by a Bounding Interface

Cited by 284 publications

References 28 publications

Glass Transition Measurements of Ultrathin Polystyrene Films

Glass Transition Measurements of Ultrathin Polystyrene Films

Structure and dynamics of poly(methyl methacrylate)/graphene systems through atomistic molecular dynamics simulations

Surface Diffusion of Poly(ethylene glycol)

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