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Mixed Self-Assembled Monolayers with Deuterated Terminal Anchors for Tethered Lipid Membrane Formation
Linköping University, Department of Physics, Chemistry and Biology. Linköping University, The Institute of Technology.
Department of Nanoengineering, Center for Physical Sciences and Technology, Savanorių 231, LT-02300 Vilnius, Lithuania.
Department of Nanoengineering, Center for Physical Sciences and Technology, Savanorių 231, LT-02300 Vilnius, Lithuania.
Department of Nanoengineering, Center for Physical Sciences and Technology, Savanorių 231, LT-02300 Vilnius, Lithuania.
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(English)Manuscript (preprint) (Other academic)
Abstract [en]

The aim of this study was to develop a stable and flexible self-assembled monolayer (SAM) for tethered lipid bilayer membrane (tBLM) formation that in the future might be employed for mimetics of more complex cell membrane architectures. Our model SAM surface conisted of a mixture of a filling molecule,  HS(CH2)15CONHCH2CH2OH, and an anchor molecule, HS(CH2)15CONH(CH2CH2O)6CH2CONH-X, where X is either –(CD2)7CD3 or – (CD2)15CD3. We have prepared and characterized their structure and chemical composition as well as the adsorption of lipids on the SAM by means of ellipsometry, contact angle goniometry, and infrared reflection-absorption spectrometry (IRRAS). The use of deuterated terminal alkyl chains enabled us to establish a correlation between the relative surface density of the anchors and the properties of the lipid bilayers formed via small unilamellar vesicle (SUV) fusion. Further on, we monitored SUV fusion kinetics on the mixed SAM  surface using quartz crystal microbalance with dissipative monitoring (QCM-D). The QCM-D analysis revealed that a critical vesicle concentration has to be reached on the SAM for vesicle rupture and bilayer formation.

National Category
Natural Sciences
Identifiers
URN: urn:nbn:se:liu:diva-77050OAI: oai:DiVA.org:liu-77050DiVA: diva2:524722
Available from: 2012-05-03 Created: 2012-05-03 Last updated: 2012-05-03
In thesis
1. Structural Studies of Oligo(ethylene glycol)-Containing Assemblies on Gold
Open this publication in new window or tab >>Structural Studies of Oligo(ethylene glycol)-Containing Assemblies on Gold
2012 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The work presents in this thesis has been focused on structural  characterization of a series of selected well-defined molecular architectures for the application as biomimetic membranes. The molecular architectures were prepared by self-assembly from dilute solution onto gold substrates, so called self-assembled monolayers (SAMs).

Biological membranes are essential components for all living systems; their molecular organizations and interactions with intra- and extracellular networks are key factors of cell functions. Many important biological processes are regulated at membrane interfaces via interactions between membrane proteins. Therefore, identification of the cell structures and understanding of the processes associated with membranes are crucial. However, the intrinsic complexity of the cell membrane systems makes direct investigation extra difficult. Based on this reason, artificial model membranes have become a useful strategy. Especially, solid supported tethered lipid membranes on SAMs allow for controlling the composition and geometry of biomimetic assemblies on molecular scale. However, the underlying mechanisms of lipid vesicle fusion on SAMs remain unclear. In this thesis, a series of thiolate SAMs containing alkyl chains and oligo(ethylene glycol) (OEG) portions of different length as well as amide linking groups were prepared and characterized in detail by employing a number of surface analyzing methods. In parallel, a set of ab initio modeling was undertaken for the best interpretation of the experimental infrared spectra. Investigation of small unilamellar vesicles interact with such SAMs is included as well.

The results show this type of assemblies forms highly ordered and oriented SAMs regardless of the length of the extended alkyl chains. The two layers of lateral hydrogen bonding networks through the two amide linking groups improve further the structural robustness of the assemblies. Furthermore, the use of deuterated terminal alkyl chains enables a direct relation between the surface density of the anchor molecules and the properties of the lipidbilayers. IRRAS data and ab initio modeling confirm that orientation of the helical OEG is affected by the second hydrogen bonding layer rather than the extended alkyl tails. Nanopatterns consisting of such SAMs with different extended alkyl chains can be employed as supports for the assembly of artificial cell membranes.

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press, 2012. 62 p.
Series
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 1446
National Category
Natural Sciences
Identifiers
urn:nbn:se:liu:diva-77056 (URN)978-91-7519-898-9 (ISBN)
Public defence
2012-05-31, Planck, Fysikhuset, Campus Valla, Linköpings universitet, Linköping, 10:15 (Swedish)
Opponent
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Available from: 2012-05-03 Created: 2012-05-03 Last updated: 2012-06-29Bibliographically approved

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Lee, Hung-HsunLiedberg, Bo

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