Using the lattice model for a liquid, we treat the packing of short-chain molecules in interhases such as bilayer membranes. The constant density in tie interphase imposes intermolecular constraints on the configurations of the flexible chains. The statistical theory here presented predicts a diffuse distribution of chain ends near the bilayer midplane; no adjustable parameters are required. Inasmuch as some of the chains terminate relatively near the polar interface, the number of chains reaching deeper planar layers is diminished. Consequently, configurational freedom increases with depth. This is the source of the well-known disorder gradient. The hydrocarbon chains in amphiphilic mesophases, such as lipid monolayers and bilayers, are highly ordered near the interfacial plane of the polar head groups. The conformations of bonds of the hydrocarbon skeleton near this interface are overwhelmingly trans in the high-temperature La phase of these systems, and the chain axes are approximately in parallel array. The order decreases with distance from the interface.The hydrophobic layer occupied by the hydrocarbon chains resembles the interphase region between lamellar crystallites and the adjoining amorphous regions in semicrystalline polymers (1), a resemblance first pointed out by deGennes (2). From the crystallite, the chains emanate with their axes normal to the lamellar surface. At this interfacial surface of the interphase the chains retain much of the order of the crystal. This order is dissipated in the interphase, as is required to conform to the disorder, virtually complete, characterizing the amorphous phase of the polymer (1).Two explanations have been offered for the gradient of disorder in lipid bilayer membranes. According to one of these, the chains near the polar heads are cooperatively tilted with respect to the bilayer normal. This inclination of the chains near the heads provides for increased volume near the midplane of the bilayer and, thus, increased disorder (3-5). Arrangement of the chains in tilted array implies correlations that are of long range; hence a close resemblance to the crystalline state should be expected. The following observations are at variance with this inference: x-ray diffraction data (6-9), the temperature coefficient of the bilayer thickness (8-10), the heat of fusion for the formation of the La phase (11), Raman spectra (12), and dilatometric measurements of the specific volume (13). Thus, intermolecular disorder resembling that in liquid paraffins is strongly indicated. Furthermore, in NMR "magic angle" experiments (14), the average chain direction is found to be coincident with the bilayer normal. In apparent contradiction, however, electron paramagnetic resonance experiments reveal a nonzero angle of tilt. This observation is presumed to arise either from perturbation of the bilayer by the electron spin probe (14,15) or from response of the electron paramagnetic resonance signal to transitory fluctuations (5).The publication costs of this article were defray...