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1.
J Am Chem Soc ; 146(37): 25544-25551, 2024 Sep 18.
Article in English | MEDLINE | ID: mdl-39214616

ABSTRACT

The fundamental question regarding the fractionation phenomenon is whether diffusion alone is responsible for it or whether an additional advection dynamic is involved. We studied the fractionation by diffusion of particles in spatially heterogeneous environments. By experimentally observing the time-sequential fractionation patterns of dye particles diffusing across a solid-solid interface of varying polyacrylamide gel densities, we found that the two-component diffusion model accurately captures the observed fractionation dynamics. In contrast, single-component diffusion models by Fick, Wereide, and Chapman do not. Our results indicate that diffusion alone can explain the fractionation phenomenon and that additional advection dynamics are not involved. The underlying physics in the fractionation phenomenon is discussed by using a two-component random walk model.

2.
J Am Chem Soc ; 146(20): 13846-13853, 2024 May 22.
Article in English | MEDLINE | ID: mdl-38652033

ABSTRACT

Lipid rafts, which are dynamic nanodomains in the plasma membrane, play a crucial role in intermembrane processes by clustering together and growing in size within the plane of the membrane while also aligning with each other across different membranes. However, the physical origin of layer by layer alignment of lipid rafts remains to be elucidated. Here, by using fluorescence imaging and synchrotron X-ray reflectivity in a phase-separated multilayer system, we find that the alignment of raft-mimicking Lo domains is regulated by the distance between bilayers. Molecular dynamics simulations reveal that the aligned state is energetically preferred when the intermembrane distance is small due to its ability to minimize the volume of surface water, which has fewer water hydrogen bonds (HBs) compared to bulk water. Our results suggest that water HB-driven alignment of lipid rafts plays a role as a precursor of intermembrane processes such as cell-cell fusion, virus entry, and signaling.


Subject(s)
Hydrogen Bonding , Membrane Microdomains , Molecular Dynamics Simulation , Water , Water/chemistry , Membrane Microdomains/chemistry , Lipid Bilayers/chemistry , Lipid Bilayers/metabolism
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