Ripple-like instability in the simulated gel phase of finite size phosphocholine bilayers

Abstract: Atomistic molecular dynamics simulations have reached a degree of maturity that makes it possible to investigate the lipid polymorphism of model bilayers over a wide range of temperatures. However if both the fluid $L_{\alpha}$ and tilted gel $L_{\beta'}$ states are routinely obtained, the $P_{\beta'}$ ripple phase of phosphatidylcholine lipid bilayers is still unsatifactorily described. Performing simulations of lipid bilayers made of different numbers of DPPC (1,2-dipalmitoylphosphatidylcholine) molecules ranging from 32 to 512, we demonstrate that the tilted gel phase $L_{\beta'}$ expected below the pre-transition cannot be obtained for large systems ($>$ 94 DPPC molecules) through common simulations settings or temperature treatments. Large systems are instead found in a disordered gel phase which display configurations, topography and energies reminiscent from the ripple phase $P_{\beta'}$ observed between the pretransition and the main melting transition. We show how the state of the bilayers below the pretransition can be controlled and depends on thermal history and conditions of preparations. A mechanism for the observed topographic instability is suggested.