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Understanding the (de)mixing behavior of multicomponent lipid bilayers is animportant step towards unraveling the nature of spatial compositionheterogeneities in cellular membranes and their role in biological function. Weuse coarse-grained molecular dynamics simulations to study the compositionphase diagram of a quaternary mixture of phospholipids and cholesterol. Thismixture is known to exhibit both uniform and coexisting phases. We compare andcombine different statistical measures of membrane structure to identify theonset of phase coexistence in composition space. An important element in ourapproach is the dependence of composition heterogeneities on the size of thesystem. While homogeneous phases can be structured and display long correlationlengths, the hallmark behavior of phase coexistence is the scaling of theapparent correlation length with system size. Because the latter cannot beeasily varied in simulations, our method instead uses information obtained fromobservation windows of different sizes to accurately distinguish phasecoexistence from structured homogeneous phases. This approach is built on verygeneral physical principles, and will be beneficial to future studies of thephase behavior of multicomponent lipid bilayers.

Identifying the Onset of Phase Separation in Quaternary Lipid Bilayer Systems from Coarse-Grained Simulations