The 2H NMR transverse relaxation rates of a deuterated phospholipid bilayer reflect slow motions in the bilayer membrane. A study of dimyristoyl lecithin specifically deuterated at several positions of the hydrocarbon chains indicates that these motions are cooperative and are confined to the hydrocarbon chains of the lipid bilayer. However, lipid head group interactions do play an important role in modulating the properties of the cooperative fluctuations of the hydrocarbon chains (director fluctuations), as evidenced by the effects of various lipid additives on the 2H NMR transverse relaxation rates of the dimyristoyl lecithin bilayer. Because liposomal bilayers are curved structures, however, the presence of significant lateral diffusion may complicate the angular dependence of T-1. If the rate of lateral diffusion is comparable to T-j', an average over X is necessary. The limits of this averaging may be expressed as,8 ± A,/, where the magnitude of Ad will depend both on the rate of lateral diffusion ofthe lipid molecules within each monolayer as well as the radius of curvature of the liposome. In the limit that lateral diffusion is complete over the time scale of T-1, (sin2(2,3)) = 16/30, and the angular dependence of T,-1 vanishes. However, when the rate of lateral diffusion is rapid compared to T-1, the physics is modified (20), the effects of director fluctuations are masked, and no angular dependence of T2-1 on p is expected.In this paper, we use the angular dependence of T, 1 and the dependence of T-j1 on the order parameter to characterize the nature of slow motions and to determine the contribution of director fluctuations to T-1 in a dimyristoyl lecithin (DML) bilayer. The effects ofdistearoyl lecithin (DSL), myristic acid (MA), cholesterol, phytol, and chlorophyll a (Chl-a) on the T-1 of the DML bilayer are also determined. The structures of these lipids are shown in Fig. 1 DML deuterated at the 9 and 10 positions on both chains ([9,9',10,10'-2H4]DML) was synthesized as described previously (4). [(2,2,2',2')-2H4]DML was synthesized by attaching MA deuterated at the 2 position to a glycerophosphocholine Abbreviations: DML, dimyristoyl lecithin; DSL, distearoyl lecithin; MA, myristic acid; Chl-a, chlorophyll a; Ti1, spin-spin relaxation rate.