Experimental evidence on the effect of substrate roughness on segmental dynamics of confined polymer films

Unni, Aparna Beena; Chat, Katarzyna; Duarte, Daniel M.; Wojtyniak, Marcin; Geppert‐Rybczyńska, Monika; Kubacki, Jerzy; Wrzalik, R.; Richert, Ranko; Adrjanowicz, Karolina

doi:10.1016/j.polymer.2020.122501

Cited by 14 publications

(31 citation statements)

References 55 publications

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“…As already noted, to extract the properties of the pure polymer film, correction of the dielectric data is needed according to the model proposed by us recently. 74 Therefore, the raw dielectric data as that presented in Figure 5 were fitted accordingly to the proposed model, assuming that the dielectric permittivity of the sample is given by the sum of the Havriliak–Negami (HN) function and a dc-conductivity term. The additional contribution seen on the high-frequency side of the spectrum is due to the nonzero resistivity of the electrodes.…”

Section: Resultsmentioning

confidence: 99%

“…The solid line shows the representative fit of the raw data according to the model described in our previous paper. 74 …”

Section: Resultsmentioning

confidence: 99%

“…This can be done according to the model introduced by us in a recent paper. 74 The model allows to distinguish the confined polymer dynamics from the total dielectric signal that is affected by the contribution coming from the nonzero resistivity of the Si electrodes, the silicon oxide isolating layer, and the spacer posts/air gap between the polymer layer and the upper electrode. The results have led to the conclusion that the most severe change in the loss peak profile in such configuration is due to the air gap that in many cases is much thicker than the polymer film itself.…”

Section: Methodsmentioning

confidence: 99%

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On the Segmental Dynamics and the Glass Transition Behavior of Poly(2-vinylpyridine) in One- and Two-Dimensional Nanometric Confinement

Winkler

Unni

et al. 2021

J. Phys. Chem. B

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Geometric nanoconfinement, in one and two dimensions, has a fundamental influence on the segmental dynamics of polymer glass-formers and can be markedly different from that observed in the bulk state. In this work, with the use of dielectric spectroscopy, we have investigated the glass transition behavior of poly(2-vinylpyridine) (P2VP) confined within alumina nanopores and prepared as a thin film supported on a silicon substrate. P2VP is known to exhibit strong, attractive interactions with confining surfaces due to the ability to form hydrogen bonds. Obtained results show no changes in the temperature evolution of the α-relaxation time in nanopores down to 20 nm size and 24 nm thin film. There is also no evidence of an out-of-equilibrium behavior observed for other glass-forming systems confined at the nanoscale. Nevertheless, in both cases, the confinement effect is seen as a substantial broadening of the α-relaxation time distribution. We discussed the results in terms of the importance of the interfacial energy between the polymer and various substrates, the sensitivity of the glass-transition temperature to density fluctuations, and the density scaling concept.

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Section: Resultsmentioning

confidence: 99%

“…The solid line shows the representative fit of the raw data according to the model described in our previous paper. 74 …”

Section: Resultsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

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On the Segmental Dynamics and the Glass Transition Behavior of Poly(2-vinylpyridine) in One- and Two-Dimensional Nanometric Confinement

Winkler

Unni

et al. 2021

J. Phys. Chem. B

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“…This generally valid idea is a good starting point in probing the structure–dynamics relation in polymer nanocomposites and films. However, due to the large number of the parameters affecting the properties and the experimental challenges related to the sample preparation [ 8 , 9 , 10 ], which in part stem from the irregularity of the surface [ 11 , 12 , 13 , 14 ], many essential theoretical questions remain to be addressed [ 15 , 16 ].…”

Section: Introductionmentioning

confidence: 99%

“…Motivated by a recent experimental interest in rough surfaces [ 11 , 12 , 13 , 14 ], we aim to provide a detailed analysis of the structure–dynamics relation in hybrid polymer-based materials with irregular interfaces. More specifically, we employ an atomistic molecular dynamics simulation technique to study a realistic model of cis -1,4-polybutadiene chains in melt adsorbed on an amorphous silica slab.…”

Section: Introductionmentioning

confidence: 99%

Coupling between Polymer Conformations and Dynamics Near Amorphous Silica Surfaces: A Direct Insight from Atomistic Simulations

Bačová

Behbahani

et al. 2021

Nanomaterials

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The dynamics of polymer chains in the polymer/solid interphase region have been a point of debate in recent years. Its understanding is the first step towards the description and the prediction of the properties of a wide family of commercially used polymeric-based nanostructured materials. Here, we present a detailed investigation of the conformational and dynamical features of unentangled and mildly entangled cis-1,4-polybutadiene melts in the vicinity of amorphous silica surface via atomistic simulations. Accounting for the roughness of the surface, we analyze the properties of the polymer chains as a function of their distance from the silica slab, their conformations and the chain molecular weight. Unlike the case of perfectly flat and homogeneous surfaces, the monomeric translational motion parallel to the surface was affected by the presence of the silica slab up to distances comparable with the extension of the density fluctuations. In addition, the intramolecular dynamical heterogeneities in adsorbed chains were revealed by linking the conformations and the structure of the adsorbed chains with their dynamical properties. Strong dynamical heterogeneities within the adsorbed layer are found, with the chains possessing longer sequences of adsorbed segments (“trains”) exhibiting slower dynamics than the adsorbed chains with short ones. Our results suggest that, apart from the density-dynamics correlation, the configurational entropy plays an important role in the dynamical response of the polymers confined between the silica slabs.

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Recent advancements in experimental methods for investigating irreversible chain adsorption at polymer-solid interfaces

Wu,

Wang,

Sun

et al. 2024

Polymer

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Experimental evidence on the effect of substrate roughness on segmental dynamics of confined polymer films

Cited by 14 publications

References 55 publications

On the Segmental Dynamics and the Glass Transition Behavior of Poly(2-vinylpyridine) in One- and Two-Dimensional Nanometric Confinement

On the Segmental Dynamics and the Glass Transition Behavior of Poly(2-vinylpyridine) in One- and Two-Dimensional Nanometric Confinement

Coupling between Polymer Conformations and Dynamics Near Amorphous Silica Surfaces: A Direct Insight from Atomistic Simulations

Recent advancements in experimental methods for investigating irreversible chain adsorption at polymer-solid interfaces

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