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      Surfactant-Mediated Structural Modulations to Planar, Amphiphilic Multilamellar Stacks

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          Abstract

          The hydrophobic effect, a ubiquitous process in biology, is a primary thermodynamic driver of amphiphilic self-assembly. It leads to the formation of unique morphologies including two highly important classes of lamellar and micellar mesophases. The interactions between these two types of structures and their involved components have garnered significant interest because of their importance in key biochemical technologies related to the isolation, purification, and reconstitution of membrane proteins. This work investigates the structural organization of mixtures of the lamellar-forming phospholipid 1-palmitoyl-2-oleoyl- sn-glycero-3-phosphocholine (POPC) and two zwitterionic micelle-forming surfactants, being n-dodecyl- N, N-dimethyl-3-ammonio-1-propanesulfonate (Zwittergent 3-12 or DDAPS) and 1-oleoyl-2-hydroxy- sn-glycero-3-phosphocholine (O-Lyso-PC), when assembled by water vapor hydration with X-ray diffraction measurements, brightfield optical microscopy, wide-field fluorescence microscopy, and atomic force microscopy. The results reveal that multilamellar mesophases of these mixtures can be assembled across a wide range of POPC to surfactant (POPC:surfactant) concentration ratios, including ratios far surpassing the classical detergent-saturation limit of POPC bilayers without significant morphological disruptions to the lamellar motif. The mixed mesophases generally decreased in lamellar spacing ( D) and headgroup-to-headgroup distance ( D hh) with a higher concentration of the doped surfactant, but trends in water layer thickness ( D w) between each bilayer in the stack are highly variable. Further structural characteristics including mesophase topography, bilayer thickness, and lamellar rupture force were revealed by atomic force microscopy (AFM), exhibiting homogeneous multilamellar stacks with no significant physical differences with changes in the surfactant concentration within the mesophases. Taken together, the outcomes present the assembly of unanticipated and highly unique mixed mesophases with varied structural trends from the involved surfactant and lipidic components. Modulations in their structural properties can be attributed to the surfactant’s chemical specificity in relation to POPC, such as the headgroup hydration and the hydrophobic chain tail mismatch. Taken together, our results illustrate how specific chemical complexities of surfactant–lipid interactions can alter the morphologies of mixed mesophases and thereby alter the kinetic pathways by which surfactants dissolve lipid mesophases in bulk aqueous solutions.

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          Most cited references75

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          Theory of self-assembly of hydrocarbon amphiphiles into micelles and bilayers

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            Self-Assembly of Colloidal Nanocrystals: From Intricate Structures to Functional Materials.

            Chemical methods developed over the past two decades enable preparation of colloidal nanocrystals with uniform size and shape. These Brownian objects readily order into superlattices. Recently, the range of accessible inorganic cores and tunable surface chemistries dramatically increased, expanding the set of nanocrystal arrangements experimentally attainable. In this review, we discuss efforts to create next-generation materials via bottom-up organization of nanocrystals with preprogrammed functionality and self-assembly instructions. This process is often driven by both interparticle interactions and the influence of the assembly environment. The introduction provides the reader with a practical overview of nanocrystal synthesis, self-assembly, and superlattice characterization. We then summarize the theory of nanocrystal interactions and examine fundamental principles governing nanocrystal self-assembly from hard and soft particle perspectives borrowed from the comparatively established fields of micrometer colloids and block copolymer assembly. We outline the extensive catalog of superlattices prepared to date using hydrocarbon-capped nanocrystals with spherical, polyhedral, rod, plate, and branched inorganic core shapes, as well as those obtained by mixing combinations thereof. We also provide an overview of structural defects in nanocrystal superlattices. We then explore the unique possibilities offered by leveraging nontraditional surface chemistries and assembly environments to control superlattice structure and produce nonbulk assemblies. We end with a discussion of the unique optical, magnetic, electronic, and catalytic properties of ordered nanocrystal superlattices, and the coming advances required to make use of this new class of solids.
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              Elastic Properties of Lipid Bilayers: Theory and Possible Experiments

              W Helfrich (1973)
              A theory of the elasticity of lipid bilayers is proposed. Three types of strain, i. e. stretching, tilt and curvature, are distinguished and the associated stresses are identified. It is argued that in the case of vesicles (= closed bilayer films) the only elasticity controlling nonspherical shapes is that of curvature. Euler-Lagrange equations are derived for the shape in magnetic fields and under excess outside pressure. It is shown that magnetic fields can deform spherical vesicles into ellipsoids of revolution. Under excess outside pressure the spherical shape becomes unstable at a certain threshold pressure. Both effects can be influenced by a spontaneous curvature of the bilayer. Some possible experiments to determine the elastic properties are also discussed
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                Author and article information

                Journal
                J Phys Chem B
                J Phys Chem B
                jp
                jpcbfk
                The Journal of Physical Chemistry. B
                American Chemical Society
                1520-6106
                1520-5207
                16 August 2023
                31 August 2023
                : 127
                : 34
                : 7497-7508
                Affiliations
                []Chemistry Graduate Group, University of California, Davis , One Shields Avenue, Davis, California 95616, United States
                []Department of Physics, University of California, San Diego , 9500 Gilman Drive, La Jolla, California 92093, United States
                [§ ]Department of Chemistry, University of California, Davis , One Shields Avenue, Davis, California 95616, United States
                []Department of Biomedical Engineering, University of California, Davis , One Shields Avenue, Davis, California 95616, United States
                Author notes
                Author information
                https://orcid.org/0000-0001-5993-9862
                https://orcid.org/0000-0002-5927-4968
                Article
                10.1021/acs.jpcb.3c01654
                10476200
                37584633
                d1034efd-1349-4318-88e6-3a930a046596
                © 2023 The Authors. Published by American Chemical Society

                Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained ( https://creativecommons.org/licenses/by/4.0/).

                History
                : 10 March 2023
                : 01 August 2023
                Funding
                Funded by: National Science Foundation, doi 10.13039/100000001;
                Award ID: DMR-2104123
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                jp3c01654
                jp3c01654

                Physical chemistry
                Physical chemistry

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