Two-dimensional X-ray diffraction (XRD) analyses of transparent mesoscopica
lly ordered silica/ block copolymer composite monoliths reveal single-cryst
al-like patterns that correspond to well-ordered hexagonal domains that are
greater than 1 cm x 1 mm x 1 mm in size. Analyses of the diffraction patte
rns reveal highly uniform hexagonal domains with narrow distributions of or
ientational order that are characterized by a phi-mosaic smaller than 2 deg
rees in the plane of the hexagonal lattice and a chi-mosaic smaller than 11
degrees along the cylindrical aggregate axes. XRD and TEM results also sho
w that the composite monoliths have large well-ordered cubic mesophase doma
ins in the meniscus regions of the samples. Boundaries between the hexagona
l and cubic domains in the monoliths reflect gradual transitions between th
e two epitaxially related structures. Such large single-domain hexagonal an
d cubic mesostructures were furthermore preserved following removal of the
organic species by calcination to produce mesoporous silica monoliths.