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Confinement Effects on Glass-Forming Aqueous Dimethyl Sulfoxide Solutions

Demuth, Dominik ; Reuhl, Melanie ; Hopfenmüller, Moritz ; Karabas, Nail ; Schoner, Simon ; Vogel, Michael (2021):
Confinement Effects on Glass-Forming Aqueous Dimethyl Sulfoxide Solutions. (Publisher's Version)
In: Molecules, 25 (18), MDPI, ISSN 1420-3049,
DOI: 10.26083/tuprints-00019243,
[Article]

Abstract

Combining broadband dielectric spectroscopy and nuclear magnetic resonance studies, we analyze the reorientation dynamics and the translational diffusion associated with the glassy slowdown of the eutectic aqueous dimethyl sulfoxide solution in nano-sized confinements, explicitly, in silica pores with different diameters and in ficoll and lysozyme matrices at different concentrations. We observe that both rotational and diffusive dynamics are slower and more heterogeneous in the confinements than in the bulk but the degree of these effects depends on the properties of the confinement and differs for the components of the solution. For the hard and the soft matrices, the slowdown and the heterogeneity become more prominent when the size of the confinement is reduced. In addition, the dynamics are more retarded for dimethyl sulfoxide than for water, implying specific guest-host interactions. Moreover, we find that the temperature dependence of the reorientation dynamics and of the translational diffusion differs in severe confinements, indicating a breakdown of the Stokes–Einstein–Debye relation. It is discussed to what extent these confinement effects can be rationalized in the framework of core-shell models, which assume bulk-like and slowed-down motions in central and interfacial confinement regions, respectively.

Item Type: Article
Erschienen: 2021
Creators: Demuth, Dominik ; Reuhl, Melanie ; Hopfenmüller, Moritz ; Karabas, Nail ; Schoner, Simon ; Vogel, Michael
Origin: Secondary publication via sponsored Golden Open Access
Status: Publisher's Version
Title: Confinement Effects on Glass-Forming Aqueous Dimethyl Sulfoxide Solutions
Language: English
Abstract:

Combining broadband dielectric spectroscopy and nuclear magnetic resonance studies, we analyze the reorientation dynamics and the translational diffusion associated with the glassy slowdown of the eutectic aqueous dimethyl sulfoxide solution in nano-sized confinements, explicitly, in silica pores with different diameters and in ficoll and lysozyme matrices at different concentrations. We observe that both rotational and diffusive dynamics are slower and more heterogeneous in the confinements than in the bulk but the degree of these effects depends on the properties of the confinement and differs for the components of the solution. For the hard and the soft matrices, the slowdown and the heterogeneity become more prominent when the size of the confinement is reduced. In addition, the dynamics are more retarded for dimethyl sulfoxide than for water, implying specific guest-host interactions. Moreover, we find that the temperature dependence of the reorientation dynamics and of the translational diffusion differs in severe confinements, indicating a breakdown of the Stokes–Einstein–Debye relation. It is discussed to what extent these confinement effects can be rationalized in the framework of core-shell models, which assume bulk-like and slowed-down motions in central and interfacial confinement regions, respectively.

Journal or Publication Title: Molecules
Journal volume: 25
Number: 18
Publisher: MDPI
Collation: 24 Seiten
Divisions: 05 Department of Physics
05 Department of Physics > Institute for Condensed Matter Physics
Date Deposited: 03 Aug 2021 07:16
DOI: 10.26083/tuprints-00019243
Official URL: https://tuprints.ulb.tu-darmstadt.de/19243
URN: urn:nbn:de:tuda-tuprints-192433
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