Schlaich, Alexander ; Daldrop, Jan O. ; Kowalik, Bartosz ; Kanduč, Matej ; Schneck, Emanuel ; Netz, Roland R. (2024)
Water Structuring Induces Nonuniversal Hydration Repulsion between Polar Surfaces: Quantitative Comparison between Molecular Simulations, Theory and Experiments.
In: Langmuir, 40 (15)
doi: 10.1021/acs.langmuir.3c03656
Artikel, Bibliographie
Dies ist die neueste Version dieses Eintrags.
Kurzbeschreibung (Abstract)
Polar surfaces in water typically repel each other at close separations, even if they are charge-neutral. This so-called hydration repulsion balances the van der Waals attraction and gives rise to a stable nanometric water layer between the polar surfaces. The resulting hydration water layer is crucial for the properties of concentrated suspensions of lipid membranes and hydrophilic particles in biology and technology, but its origin is unclear. It has been suggested that surface-induced molecular water structuring is responsible for the hydration repulsion, but a quantitative proof of this water-structuring hypothesis is missing. To gain an understanding of the mechanism causing hydration repulsion, we perform molecular simulations of different planar polar surfaces in water. Our simulated hydration forces between phospholipid bilayers agree perfectly with experiments, validating the simulation model and methods. For the comparison with theory, it is important to split the simulated total surface interaction force into a direct contribution from surface–surface molecular interactions and an indirect water-mediated contribution. We find the indirect hydration force and the structural water-ordering profiles from the simulations to be in perfect agreement with the predictions from theoretical models that account for the surface-induced water ordering, which strongly supports the water-structuring hypothesis for the hydration force. However, the comparison between the simulations for polar surfaces with different headgroup architectures reveals significantly different decay lengths of the indirect water-mediated hydration-force, which for laterally homogeneous water structuring would imply different bulk-water properties. We conclude that laterally inhomogeneous water ordering, induced by laterally inhomogeneous surface structures, shapes the hydration repulsion between polar surfaces in a decisive manner. Thus, the indirect water-mediated part of the hydration repulsion is caused by surface-induced water structuring but is surface-specific and thus nonuniversal.
| Typ des Eintrags: | Artikel |
|---|---|
| Erschienen: | 2024 |
| Autor(en): | Schlaich, Alexander ; Daldrop, Jan O. ; Kowalik, Bartosz ; Kanduč, Matej ; Schneck, Emanuel ; Netz, Roland R. |
| Art des Eintrags: | Bibliographie |
| Titel: | Water Structuring Induces Nonuniversal Hydration Repulsion between Polar Surfaces: Quantitative Comparison between Molecular Simulations, Theory and Experiments |
| Sprache: | Englisch |
| Publikationsjahr: | 5 April 2024 |
| Ort: | Washington, DC |
| Verlag: | American Chemical Society |
| Titel der Zeitschrift, Zeitung oder Schriftenreihe: | Langmuir |
| Jahrgang/Volume einer Zeitschrift: | 40 |
| (Heft-)Nummer: | 15 |
| DOI: | 10.1021/acs.langmuir.3c03656 |
| Zugehörige Links: | |
| Kurzbeschreibung (Abstract): | Polar surfaces in water typically repel each other at close separations, even if they are charge-neutral. This so-called hydration repulsion balances the van der Waals attraction and gives rise to a stable nanometric water layer between the polar surfaces. The resulting hydration water layer is crucial for the properties of concentrated suspensions of lipid membranes and hydrophilic particles in biology and technology, but its origin is unclear. It has been suggested that surface-induced molecular water structuring is responsible for the hydration repulsion, but a quantitative proof of this water-structuring hypothesis is missing. To gain an understanding of the mechanism causing hydration repulsion, we perform molecular simulations of different planar polar surfaces in water. Our simulated hydration forces between phospholipid bilayers agree perfectly with experiments, validating the simulation model and methods. For the comparison with theory, it is important to split the simulated total surface interaction force into a direct contribution from surface–surface molecular interactions and an indirect water-mediated contribution. We find the indirect hydration force and the structural water-ordering profiles from the simulations to be in perfect agreement with the predictions from theoretical models that account for the surface-induced water ordering, which strongly supports the water-structuring hypothesis for the hydration force. However, the comparison between the simulations for polar surfaces with different headgroup architectures reveals significantly different decay lengths of the indirect water-mediated hydration-force, which for laterally homogeneous water structuring would imply different bulk-water properties. We conclude that laterally inhomogeneous water ordering, induced by laterally inhomogeneous surface structures, shapes the hydration repulsion between polar surfaces in a decisive manner. Thus, the indirect water-mediated part of the hydration repulsion is caused by surface-induced water structuring but is surface-specific and thus nonuniversal. |
| Freie Schlagworte: | Hydration, Order, Polarization, Vesicles, Water |
| Zusätzliche Informationen: | Published as part of Langmuir virtual special issue “Highlighting Contributions from our Editorial Board Members in 2023”. |
| Sachgruppe der Dewey Dezimalklassifikatin (DDC): | 500 Naturwissenschaften und Mathematik > 530 Physik 500 Naturwissenschaften und Mathematik > 540 Chemie |
| Fachbereich(e)/-gebiet(e): | 05 Fachbereich Physik 05 Fachbereich Physik > Institut für Physik Kondensierter Materie (IPKM) 05 Fachbereich Physik > Institut für Physik Kondensierter Materie (IPKM) > Physik biologischer weicher Materie |
| Hinterlegungsdatum: | 16 Mai 2024 14:59 |
| Letzte Änderung: | 16 Mai 2024 14:59 |
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Verfügbare Versionen dieses Eintrags
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Water Structuring Induces Nonuniversal Hydration Repulsion between Polar Surfaces: Quantitative Comparison between Molecular Simulations, Theory and Experiments. (deposited 13 Mai 2024 13:27)
- Water Structuring Induces Nonuniversal Hydration Repulsion between Polar Surfaces: Quantitative Comparison between Molecular Simulations, Theory and Experiments. (deposited 16 Mai 2024 14:59) [Gegenwärtig angezeigt]
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