BARC/PUB/2018/1224

 
 

Heterogeneity in Dynamics of Dioctadecyldimethylammonium Bromide Bilayers: Molecular Dynamics Simulation and Neutron Scattering Study

 
     
 
Author(s)

Srinivasan, H.; Sharma, V. K.; Mitra, S.; Mukhopadhyay, R.
(SSPD)

Source

Journal of Physical Chemistry-C, 2018. Vol. 122: pp. 20419-20430

ABSTRACT

Molecular dynamics (MD) simulations have been carried out to investigate the structural and dynamical aspects of dioctadecyldimethylammonium bromide (DODAB) bilayer which exists in various phases. MD simulation at 300 K shows that the bilayer system is found to form an asymmetric ripple phase with highly ordered and tightly packed alkyl chains. While at 350 K, the system is found to be in the fluid phase, marked by a significant increase in fluidity and in the presence of significant gauche defects. Alkyl chain order parameter suggests that ordering is highest near the headgroup region in both the phases. The mean squared displacement corresponding to the lateral motion of DODAB lipid scales as tα, with α ∼0.5 at 300 K and ∼0.62 at 350 K, indicating subdiffusive motion, which is modeled in the framework of generalized Langevin equation (GLE). It is also found that the lateral motion of the lipid is spatially homogenous; hence, the origin of subdiffusive process is temporal heterogeneity which is captured by the memory function obtained from GLE. High energy resolution neutron scattering data recorded on the same system are analyzed by comparing the incoherent intermediate scattering function (IISF) calculated from simulation. IISF are analyzed assuming three independent dynamical processes lateral, segmental, and torsional motion of the lipids. Here too, the lateral motion is found to be well described by a spatially homogenous subdiffusive motion. The segmental dynamics of the alkyl chain is delineated successfully using the localized translational diffusion model, where the variation of dynamicity along the alkyl chain is in compliance with the internal dynamics observed in the MD simulation. The torsional motion is described by twofold rotation. This work describes the complex dynamical behavior of DODAB lipid bilayer using MD simulation and neutron scattering studies consistently. The understanding of dynamics of DODAB bilayer would be useful in various applications including DNA/gene transfection and drug transport.

 
 
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