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Mixtures of cetyltrimethylammonium tosylate (CTAT) and sodium dodecylbenzene sulfonate (SDBS) in water form a fluid lamellar phase at < or = 40 wt % water but surprisingly turn into viscous gels at higher water fractions. The gels are characterized by spherulite and other bilayer defects consistent with a low bending elasticity, kappa approximately k(B)T, and a nonzero spontaneous curvature. Caillé analysis of the small-angle x-ray line shape confirms that for 7:3 wt:wt CTAT:SDBS bilayers at 50% water, kappa = 0.62 +/- 0.09 k(B)T and kappa = -0.9 +/- 0.2 k(B)T. For 13:7 wt:wt CTAT:SDBS bilayers, the measured bending elasticity decreases with increasing water dilution in good agreement with predictions based on renormalization theory, giving kappa(o) = 0.28 k(B)T. These results show that surfactant mixing is sufficient to make kappa approximately k(B)T, which promotes strong, Helfrich-type repulsion between bilayers that can dominate the van der Waals attraction. These are necessary conditions for spontaneous vesicles formed at even higher water fractions to be equilibrium structures.

A transient metastable rotator phase occurring on crystallization of hexadecane into its triclinic phase from the supercooled melt was directly observed with time-resolved synchrotron x-ray scattering. In this system, the limit of supercooling (the crystallization temperature) is determined by the thermodynamic stability of the transient phase with respect to the liquid. The crystallization kinetics of the homologous series of n-alkanes was measured and explained in terms of a crossover from stability to "long-lived" metastability to transient metastability. This crossover allowed further confirmation of the nature of the transient phase.

Surface tension measurements reveal surface freezing in liquid n-alkanes. A solid monolayer of molecules is found to exist up to 30 degrees C above the bulk freezing point. This surface phase exists only for carbon numbers 14 n

Synchrotron x-ray scattering studies were performed to probe the nonequilibrium structures of two layered systems at high shear rates: the smectic-A phase of the thermotropic liquid crystal 4-cyano-4'-octylbiphenyl (8CB) and the lamellar L(alpha) phases of surfactant membranes composed of sodium dodecyl sulfate and pentanol. Whereas the lamellar surfactant phases oriented primarily with their layers parallel to the shearing plates, as expected intuitively, in the corresponding high shear regime, the smectic-A liquid crystalline material oriented with the layers perpendicular to the shearing plates. A careful numerical study revealed that this surprising layer orientation results from nonlinear dynamics of the liquid crystal director and is caused by the flow distortion of thermal fluctuations.

X-ray scattering studies were performed to understand the structure and correlations in the lamellar phases of thick, freely suspeded films of (i) the hydrated phospholipid dimyristoylphosphotidylcholine (DMPC) and (ii) the ternar system consisting of the surfactant sodium dodecyl sulfate (SDS), cosurfactant (pentanol), and water. The films were drawn in a temperature- and humidity-controlled environment, where the layers were oriented to within 0.1 degrees . In the DMPC system, this made it possible to directly observe the orientation of the P(beta') modulation and to identify phase L(beta') as three distinct phases distinguished by the direction of chain tilt with respect to the lattice. In the L(alpha) phase of the ternary system, power law behavior of the (0,0,L) structure factor arising from the algebraic decay of layer correlatios was observed in single crystals.