Gel-Phase-like Ordered Membrane Properties Observed in Dispersed Oleic Acid/1-Oleoylglycerol Self-Assemblies: Systematic Characterization Using Raman Spectroscopy and a Laurdan Fluorescent Probe

Langmuir : the ACS Journal of Surfaces and Colloids
Keishi SugaHiroshi Umakoshi

Abstract

Aqueous dispersions of oleic acid (OA) and those modified with 1-oleoylglycerol (monoolein, MO) form various kinds of self-assembled structures: micelles, vesicles, oil-in-water (O/W) emulsions, hexagonal phases, and dispersed cubic phases. Conventionally, these self-assembled structures have been characterized using cryogenic transmission electron microscopy or X-ray diffraction spectroscopy. However, these methodologies require specialized treatment before they can be used, which may lead to the self-assemblies not adopting their true equilibrium state. Herein, we systematically characterized the self-assemblies composed of OA and MO in aqueous solution using Raman spectroscopy and fluorescent probe 6-dodecanoyl-2-dimethylaminonaphthalene (Laurdan). The OA/MO dispersions at pH 5.0 showed increased chain packing in comparison to the OA micelle at pH 11 or OA vesicle at pH 9.0, which were characterized by the intensity ratio of the Raman peaks at 2850 and 2890 cm-1, R = I2890/I2850. In the Laurdan fluorescence measurements, the obtained spectra were deconvoluted to two peak fractions (A1: λem= 490 nm; A2: λem = 440 nm), and the peak area ratio, A1/(A1 + A2), was defined as the membrane hydrophilicity Øm. The Øm value of the OA/...Continue Reading

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