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Anomalous Diffusion in a Gel-Fluid Lipid Environment: A Combined Solid-State NMR and Obstructed Random-Walk Perspective

Département de Chimie, Centre de Recherche en Sciences et Ingénierie des Macromolécules, Université Laval, Québec, Canada

Correspondence: Address reprint requests to Michèle Auger, Département de Chimie, CERSIM, Université Laval, Québec, Canada, G1K 7P4. Tel.: 418-656-3393, Fax: 418-656-7916, E-mail: michele.auger{at}chm.ulaval.ca.

Lateral diffusion is an essential process for the functioning of biological membranes. Solid-state nuclear magnetic resonance (NMR) is, a priori, a well-suited technique to study lateral diffusion within a heterogeneous environment such as the cell membrane. Moreover, restriction of lateral motions by lateral heterogeneities can be used as a means to characterize their geometry. The goal of this work is to understand the advantages and limitations of solid-state NMR exchange experiments in the study of obstructed lateral diffusion in model membranes. For this purpose, simulations of lateral diffusion on a sphere with varying numbers and sizes of immobile obstacles and different percolation properties were performed. From the results of these simulations, two-dimensional ³¹P NMR exchange maps and time-dependent autocorrelation functions were calculated. The results indicate that the technique is highly sensitive to percolation properties, total obstacle area, and, within certain limits, obstacle size. A practical example is shown, namely the study of the well-characterized DMPC-DSPC binary mixture. The comparison of experimental and simulated results yielded obstacle sizes in the range of hundreds of nanometers, therefore bridging the gap between previously published NMR and fluorescence recovery after photobleaching results. The method could also be applied to the study of membrane protein lateral diffusion in model membranes.

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