Multilamellar Structures Induced by Hydrophilic and Hydrophobic Ions Added to a Binary Mixture of D2O and 3-Methylpyridine

A phase transition is observed between a one-phase disordered phase and an ordered phase with multilamellar (onion) structures in an off-critical mixture of D2O and 3-methylpyridine (3MP) containing 85 mM of a salt in the absence of a surfactant. The salt consists of hydrophilic cations and hydrophobic anions that interact asymmetrically with the solvent composition fluctuations inducing mesophases. The structure factor of the composition distribution obtained from small-angle neutron scattering has a peak at an intermediate wave number in the disordered phase and multiple peaks in the ordered phase. Lamellar layers forming onions are composed of solvation-induced charged membranes swollen by D2O. The onion phase is realized only for small volume fractions of 3MP (in D2O-rich solvent).