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Biophys J, August 2002, p. 1014-1025, Vol. 83, No. 2
Department of Physics, Texas Tech University, Lubbock, Texas 79409 USA
Experimental evidences have indicated that cholesterol
may adapt highly regular lateral distributions (i.e., superlattices) in
a phospholipid bilayer. We investigated the formations of superlattices at cholesterol mole fraction of 0.154, 0.25, 0.40, and 0.5 using Monte
Carlo simulation. We found that in general, conventional pairwise-additive interactions cannot produce superlattices. Instead, a
multibody (nonpairwise) interaction is required. Cholesterol superlattice formation reveals that although the overall interaction between cholesterol and phospholipids is favorable, it contains two
large opposing components: an interaction favoring
cholesterol-phospholipid mixing and an unfavorable acyl chain multibody
interaction that increases nonlinearly with the number of cholesterol
contacts. The magnitudes of interactions are in the order of kT. The
physical origins of these interactions can be explained by our umbrella model. They most likely come from the requirement for polar
phospholipid headgroups to cover the nonpolar cholesterol to avoid the
exposure of cholesterol to water and from the sharp decreasing of acyl chain conformation entropy due to cholesterol contact. This study together with our previous work demonstrate that the driving force of
cholesterol-phospholipid mixing is a hydrophobic interaction, and
multibody interactions dominate others over a wide range of cholesterol concentration.
Biophys J, August 2002, p. 1014-1025, Vol. 83, No. 2
© 2002 by the Biophysical Society 0006-3495/02/08/1014/12 $2.00
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