Spatial modulation of water ordering in lecithin bilayers. Evidence for a ripple-ripple phase transition.

Intense motional averaging effects on the 2H nuclear magnetic resonance (NMR) spectrum of 2H2O that occur in aqueous dispersions of dimyristoyl-sn-glycero-3-phosphocholine (Myr2-PtdCho) are explained by a spatial modulation in the orientational order of the water induced by ripplelike structures. The ratio of the amplitude to the periodic length of the ripples, A/lambda, at a molar ratio of water/Myr2-PtdCho of 9.5:1, is measured by 2H NMR and found to be consistent with x-ray measurements of this ratio in the P beta phase of dipalmitoyl-sn-glycero-3-phosphocholine (Pam2-PtdCho) bilayers. The sensitivity of 2H NMR allows us to report the presence of two distinct ripple phases mediated with a discontinuous change in the value of A/lambda. This result suggests that the two ripple structures observed for several phospholipid systems in excess water by freeze-fracture electron microscopy may be associated with two different phases instead of the same phase as previously assumed.