Methods in the SI) distinguishes "core" chains encapsulated in the clusters, "edge" chains mainly at cluster edges, and "free" chains that are excluded from the clusters (see Fig. for demonstration). The mean deuterium order parameter (S CD ), shown in Fig. , demonstrates that "core" chains are the most ordered at all temperatures. Notably, they are also the furthest (0.90 nm) away from CHOL molecules. The "free" chains are the least ordered and closest to a CHOL (0.62 nm), whereas "edge" chains show intermediate behavior. As shown in Fig. , the "core" chains are also the least tilted, followed by the "edge" chains and finally the "free" chains. The temperature dependence of both S CD and chain tilt consist of two factors, as demonstrated in Figs. and: The "core", "edge", and "free" chain populations depend on temperature with the "core" fraction declining rapidly after T co , corresponding to the melting of the clusters. Moreover, while "free" chains show continuous change in ordering and tilt, there is a crossover in the values of the "core" and "edge" chains at T co . These two factors contribute to the striking change of slope in the temperature dependence of these properties in Fig. .