A novel structural framework is presented to rationalize the foam film stability of polyelectrolyte/surfactant mixtures using neutron reflectivity data. Provision of electrostatic or steric stabilization in thin foam films is related to the spatial distributions of molecules interacting from opposing air/water interfaces. The advance is discussed in the context of many studies on mixed systems over two decades that focused on macroscopic properties such as the surface tension, elasticity, potential and composition, but for which no robust correlations have been established. This concept can now be broadened to other colloidal dispersions of high impact for technical, environmental and life science applications.
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