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- Bergendal, Erik, et al.
(författare)
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3D texturing of the air-water interface by biomimetic self-assembly
- 2020
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Ingår i: Nanoscale Horizons. - : Royal Society of Chemistry. - 2055-6764 .- 2055-6756. ; 5:5, s. 839-846
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Tidskriftsartikel (refereegranskat)abstract
- A simple, insoluble monolayer of fatty acid is shown to induce 3D nanotexturing of the air-water interface. This advance has been achieved through the study of monolayers of a methyl-branched long chain fatty acid, analogous to those found on the surface of hair and wool, directly at the air-water interface. Specular neutron reflectometry combined with AFM probing of deposited monolayers shows pronounced 3D surface domains, which are absent for unbranched analogues and are attributed to hydrocarbon packing constraints. The resulting surface topographies of the water far exceed the height perturbation that can be explained by the presence of capillary waves of a free liquid surface. These have hitherto been considered the only source of perturbation of the flatness of a planar water interface under gravity in the absence of topographical features from the presence of extended, globular or particulate matter. This amounts to a paradigm shift in the study of interfacial films and opens the possibility of 3D texturing of the air-water interface.
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2. |
- Bergendal, Erik, et al.
(författare)
-
3D texturing of the air–water interface by biomimetic self-assembly
- 2020
-
Ingår i: Nanoscale Horizons. - 2055-6764 .- 2055-6756. ; :5, s. 839-846
-
Tidskriftsartikel (refereegranskat)abstract
- A simple, insoluble monolayer of fatty acid is shown to induce 3D nanotexturing of the air–water interface. This advance has been achieved through the study of monolayers of a methyl-branched long chain fatty acid, analogous to those found on the surface of hair and wool, directly at the air–water interface. Specular neutron reflectometry combined with AFM probing of deposited monolayers shows pronounced 3D surface domains, which are absent for unbranched analogues and are attributed to hydrocarbon packing constraints. The resulting surface topographies of the water far exceed the height perturbation that can be explained by the presence of capillary waves of a free liquid surface. These have hitherto been considered the only source of perturbation of the flatness of a planar water interface under gravity in the absence of topographical features from the presence of extended, globular or particulate matter. This amounts to a paradigm shift in the study of interfacial films and opens the possibility of 3D texturing of the air–water interface.
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3. |
- Bergendal, Erik
(författare)
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Fatty Acid Self-Assembly at the Air–Water Interface : Curvature, Patterning, and Biomimetics: A Study by Neutron Reflectometry and Atomic Force Microscopy
- 2020
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- For more than a hundred years of interfacial science, long chain fatty acids have been the primary system for the study of floating monolayers at the air–water interface due to their amphiphilic nature and system simplicity: an insoluble hydrocarbon chain and a soluble carboxyl group at a flat air–water interface. Despite―or perhaps rather due to―the assumed simplicity of such systems and the maturity of the research field, the seemingly fundamentally rooted notion of a two-dimensional water surface has yet to be challenged.The naturally occurring methyl-branched long chain fatty acid 18-methyleicosanoic acid and one of its isomers form monolayers consisting of monodisperse domains of tens of nanometres, varying in size with the placement of the methyl branch. The ability of domain-forming monolayers to three-dimensionally texture the air–water interface is investigated as a result of hydrocarbon packing constraints owing to the methyl branch.In this work, neutron reflectometry has been used to study monolayers of branched long chain fatty acids directly at the air–water interface, which allowed precise probing of how a deformable water surface is affected by monolayer structure. Such films were also transferred by Langmuir–Blodgett deposition to the air–solid interface, and subsequently imaged by atomic force microscopy. Combined, the results unanimously―and all but unambiguously―show that the self-assembly of branched long chain fatty acids texture the air–water interface, inducing domain formation by a local curvature of the water surface, and thus controverting the preconceived notion of a planar air–water interface. The size and shape of the observed domains are shown to be tuneable using three different parameters: in mixed systems of branched and unbranched fatty acids, with varying hydrocarbon length of the straight chain, and altering subphase electrolyte properties. Each of these factors effectively allows changing the local curvature of the monolayer, much like analogous three-dimensional systems in bulk lyotropic crystals. This precise tuneability opens up for sustainable nanopatterning. Finally, the results lead to a plausible hypothesis of self-healing properties as to why the surface of hair and wool have a significant proportion of branched fatty acid.
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6. |
- Bergendal, Erik, et al.
(författare)
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Tuneable interfacial surfactant aggregates mimic lyotropic phases and facilitate large scale nanopatterning
- 2021
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Ingår i: Nanoscale. - : Royal Society of Chemistry. - 2040-3364 .- 2040-3372. ; 13:1, s. 371-379
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Tidskriftsartikel (refereegranskat)abstract
- It is shown that the air-liquid interface can be made to display the same rich curvature phenomena as common lyotropic liquid crystal systems. Through mixing an insoluble, naturally occurring, branched fatty acid, with an unbranched fatty acid of the same length, systematic variation in the packing constraints at the air-water interface could be obtained. The combination of atomic force microscopy and neutron reflectometry is used to demonstrate that the water surface exhibits significant tuneable topography. By systematic variation of the two fatty acid proportions, ordered arrays of monodisperse spherical caps, cylindrical sections, and a mesh phase are all observed, as well as the expected lamellar structure. The tuneable deformability of the air-water interface permits this hitherto unexplored topological diversity, which is analogous to the phase elaboration displayed by amphiphiles in solution. It offers a wealth of novel possibilities for the tailoring of nanostructure
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8. |
- Bergendal, Erik, et al.
(författare)
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Unveiling Texture and Topography of Fatty Acid Langmuir Films : Domain Stability and Isotherm Analysis
- 2024
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Ingår i: Langmuir. - : American Chemical Society (ACS). - 0743-7463 .- 1520-5827. ; 40:20, s. 10468-10476
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Tidskriftsartikel (refereegranskat)abstract
- 3D texturing by self-assembly at the air-water interface has recently been proposed. The hypothesis of this work is that, if this is true, such domain formation should be inferable directly from pressure-area isotherms and be thermodynamically stable. Monolayers of branched fatty acid mixtures with straight chain analogues and their stability are thus studied using a combination of pressure-area isotherms, thermodynamic analysis, in situ Brewster angle microscopy, and atomic force microscopy of both LB-deposited and drop-cast films on silicon wafers. Isotherms reflecting the behavior of monodisperse 3D domains are shown to be independent of compression rate and display long-term stability. Gibbs analysis further confirms the thermodynamic rather than kinetic origin of such novel species by revealing that deviations from ideal mixing can be explained only a priori by differences in the topography of the water surface, thus also indirectly confirming the self-assembly deformation of the water interface. The intrinsic self-assembly curvature and miscibility of the two fatty acids is confirmed by drop-casting, which also provides a rapid, tunable thin-film preparation approach. Finally, the longevity of the nanostructured films is extraordinary, the long-range order of the deposited films increases with equilibration time at the water interface, and the integrity of the nanopatterns remains intact on the scale of years.
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9. |
- Bergendal, Erik, et al.
(författare)
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Unveiling Texture and Topography of Fatty Acid Langmuir Films : Domain Stability and Isotherm Analysis
- 2024
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Ingår i: Langmuir. - : American Chemical Society. - 0743-7463 .- 1520-5827. ; 40:20, s. 10468-10476
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Tidskriftsartikel (refereegranskat)abstract
- 3D texturing by self-assembly at the air-water interface has recently been proposed. The hypothesis of this work is that, if this is true, such domain formation should be inferable directly from pressure-area isotherms and be thermodynamically stable. Monolayers of branched fatty acid mixtures with straight chain analogues and their stability are thus studied using a combination of pressure-area isotherms, thermodynamic analysis, in situ Brewster angle microscopy, and atomic force microscopy of both LB-deposited and drop-cast films on silicon wafers. Isotherms reflecting the behavior of monodisperse 3D domains are shown to be independent of compression rate and display long-term stability. Gibbs analysis further confirms the thermodynamic rather than kinetic origin of such novel species by revealing that deviations from ideal mixing can be explained only a priori by differences in the topography of the water surface, thus also indirectly confirming the self-assembly deformation of the water interface. The intrinsic self-assembly curvature and miscibility of the two fatty acids is confirmed by drop-casting, which also provides a rapid, tunable thin-film preparation approach. Finally, the longevity of the nanostructured films is extraordinary, the long-range order of the deposited films increases with equilibration time at the water interface, and the integrity of the nanopatterns remains intact on the scale of years.
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