Photosensitive films incorporating molecular photoacid generators compartme
ntalized within a silica-surfactant mesophase were prepared by an evaporati
on-induced self-assembly process. Ultraviolet exposure promoted localized a
cid-catalyzed siloxane condensation, which can be used for selective etchin
g of unexposed regions; for "gray-scale" patterning of refractive index, po
re size, surface area, and wetting behavior; and for optically defining a m
esophase transformation (from hexagonal to tetragonal) within the film. The
ability to optically define and continuously central both structure and fu
nction on the macro- and mesoscales is of interest for sensor arrays, nanor
eactors, photonic and fluidic devices, and low-dielectric-constant films.