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Mixed Self-Assembled Monolayers with Terminal Deuterated Anchors: Characterization and Probing of Model Lipid Membrane Formation
Linköping University, Department of Physics, Chemistry and Biology, Molecular Physics. Linköping University, Faculty of Science & Engineering.
Department of Nanoengineering, Center for Physical Sciences and Technology, Vilnius, Lithuania.
Department of Nanoengineering, Center for Physical Sciences and Technology, Vilnius, Lithuania.
Department of Nanoengineering, Center for Physical Sciences and Technology, Vilnius, Lithuania.
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2018 (English)In: Journal of Physical Chemistry B, ISSN 1520-6106, E-ISSN 1520-5207, Vol. 122, no 34, p. 8201-8210Article in journal (Refereed) Published
Abstract [en]

We describe herein a series of self-assembled monolayers (SAMs) on gold designed for adjustable tethering of model lipid membrane phases. The SAMs consist of deuterated aliphatic anchors, HS(CH2)(15)CONH-(CH2CH2O)(6)CH2CONH-X, where X is either -(CD2)(7)CD3 or -(CD2)(15)CD3, dispersed in a stable matrix of( )protein-repellent molecules, HS(CH2)(15)CONHCH2CH2OH. The mixed SAMs with variable surface densities of the anchors are thoroughly characterized before and after adsorption of phospholipids by means of ellipsometry, contact angle goniometry, and infrared reflection-absorption spectroscopy (IRRAS). In all cases, the bottom portions of the mixed SAMs (i.e., the h-alkyl thiol segments of the molecules) are arranged in a highly ordered all-trans conformation stabilized by a network of lateral hydrogen bonds. The terminal portions of the anchors (the oligo(ethylene glycol) spacer and deuterated alkyl segments, respectively), however, possess less ordered conformations in the mixed composition regime. For the SAMs containing the longer anchors (-(CD2)(15)CD3), the contact angle and infrared data point toward partial phase segregation. These findings are in excellent agreement with molecular dynamics simulations by Schulze and Stein. Upon analysis in air, the IRRAS data also indicate strong interaction between the adsorbed phospholipid molecules and the d-alkyl tails of the mixed SAM constituents. In such assemblies are the alkyl tails of the phospholipids aligned perpendicularly with respect to the supporting substrate, regardless of the anchor length. We also probed the in situ formation of a tethered bilayer lipid membrane (tBLM) via fusion of small unilamellar vesicles (SUVs) on the characterized SAMs using a quartz crystal microbalance with dissipation monitoring. Our experiments show that SUVs fuse efficiently of the two mixed SAMs with and without a pre-adsorbed lipid layer. Owing to the defined molecular composition and phase behavior, our SAM platform is attractive for detailed studies of tBLM formation and cell mimetic applications.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2018. Vol. 122, no 34, p. 8201-8210
National Category
Physical Chemistry
Identifiers
URN: urn:nbn:se:liu:diva-151501DOI: 10.1021/acs.jpcb.8b05097ISI: 000443922600010PubMedID: 30085662Scopus ID: 2-s2.0-85052322841OAI: oai:DiVA.org:liu-151501DiVA, id: diva2:1250633
Note

Funding Agencies|Swedish Institute through the Visby program; Research Council of Lithuania [MOS-6/2010]

Available from: 2018-09-24 Created: 2018-09-24 Last updated: 2018-10-02Bibliographically approved

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Lee, Hung-Hsun

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