title: Quantifying the Heterogeneous Dynamics of a Simulated Dipalmitoylphosphatidylcholine (DPPC) Membrane.
abstract: Heterogeneity of dynamics plays a vital role in membrane function, but the methods for quantifying this heterogeneity are still being developed. Here we examine membrane dynamical heterogeneity via molecular simulations of a single-component dipalmitoylphosphatidylcholine (DPPC) lipid bilayer using the MARTINI force field. We draw upon well-established analysis methods developed in the study of glass-forming fluids and find significant changes in lipid dynamics between the fluid (Lα), and gel (Lβ) phases. In particular, we distinguish two mobility groups in the more ordered Lβ phase: (i) lipids that are transiently trapped by their neighbors and (ii) lipids with displacements on the scale of the intermolecular spacing. These distinct mobility groups spatially segregate, forming dynamic clusters that have characteristic time (1-2 μs) and length (1-10 nm) scales comparable to those of proteins and other biomolecules. We suggest that these dynamic clusters could couple to biomolecules within the membrane and thus may play a role in many membrane functions. In the equilibrium membrane, lipid molecules dynamically exchange between the mobility groups, and the resulting clusters are not associated with a thermodynamic phase separation. Dynamical clusters having similar characteristics arise in many other condensed phase materials, placing membranes in a broad class of materials with strong intermolecular interactions.
authors.forename: Neha
authors.initials: N
authors.lastname: Shafique
authors.forename: Kiley E
authors.initials: KE
authors.lastname: Kennedy
authors.affiliation: Materials Science and Engineering Division, National Institute of Standards and Technology , Gaithersburg, Maryland 20899, United States.
authors.forename: Jack F
authors.initials: JF
authors.lastname: Douglas
authors.forename: Francis W
authors.initials: FW
authors.lastname: Starr
mesh_terms: D015060:1,2-Dipalmitoylphosphatidylcholine / Q000737:chemistry*; D005782:Gels / Q000737:chemistry; D008051:Lipid Bilayers / Q000737:chemistry*; D056004:Molecular Dynamics Simulation; D013816:Thermodynamics
chemical_list: D005782:Gels; D008051:Lipid Bilayers; D015060:1,2-Dipalmitoylphosphatidylcholine