title: The dynamic stress responses to area change in planar lipid bilayer membranes.
abstract: The viscoelastic properties of planar phospholipid (dimyristoylphosphatidylcholine) bilayer membranes at 308 K are studied, many of them for the first time, using the nonequilibrium molecular dynamics simulation (NEMD) method for membrane area change. First, we present a unified formulation of the intrinsic three-dimensional (3D) and apparent in-plane viscoelastic moduli associated with area change based on the constitutive relations for a uniaxial system. The NEMD simulations of oscillatory area change process are then used to obtain the frequency-domain moduli. In the 4-250 GHz range, the intrinsic 3D elastic moduli of 20-27 kbar and viscous moduli of 0.2-9 kbar are found with anisotropy and monotonic frequency dispersion. In contrast, the apparent in-plane elastic moduli (1-9 kbar) are much smaller than, and the viscous moduli (2-6 kbar) comparable to, their 3D counterparts, due to the interplay between the lateral and normal relaxations. The time-domain relaxation functions, separately obtained by applying stepwise strains, can be fit by 4-6 exponential decay modes spanning subpicosecond to nanosecond timescale and are consistent with the frequency-domain results. From NEMD with varying strain amplitude, the linear constitutive model is shown to be valid up to 6 and 20% area change for the intrinsic 3D elastic and viscous responses, respectively, and up to 20% area change for the apparent in-plane viscoelasticity. Inclusion of a gramicidin A dimer (approximately 1 mol %) yields similar response properties with possibly smaller (<10%) viscous moduli. Our results agree well with available data from ultrasonic experiments, and demonstrate that the third dimension (thickness) of the planar lipid bilayer is integral to the in-plane viscoelasticity.
authors.affiliation: Department of Chemistry and Center for Biophysical Modeling and Simulation, University of Utah, Salt Lake City, Utah 84112-0850, USA.
authors.forename: Jonggu
authors.initials: J
authors.lastname: Jeon
authors.forename: Gregory A
authors.initials: GA
authors.lastname: Voth
mesh_terms: D004134:Dimyristoylphosphatidylcholine / Q000737:chemistry*; D004548:Elasticity; D007700:Kinetics; D016014:Linear Models; D008051:Lipid Bilayers / Q000737:chemistry*; D008560:Membrane Fluidity; D008567:Membranes, Artificial; D008956:Models, Chemical; D008958:Models, Molecular; D015233:Models, Statistical; D009038:Motion; D009991:Oscillometry / Q000379:methods; D010812:Physical Stimulation / Q000379:methods; D013314:Stress, Mechanical; D013500:Surface Tension
chemical_list: D008051:Lipid Bilayers; D008567:Membranes, Artificial; D004134:Dimyristoylphosphatidylcholine