A tough challenge in nanomaterials chemistry is the determination of the structure of multicomponent nanosystems. Dye-zeolite L composites are building blocks of hierarchically organized multifunctional materials for technological applications. Supramolecular organization inside zeolite L nanochannels, which governs electronic properties, is barely understood. This is especially true for confined close-packed dye molecules, a regime not investigated in applications yet and that might have great potential for future development in this field. Here we realize for the first time composites of zeolite L with maximally-packed fluorenone molecules and elucidate their structure by integrated multi-technique analyses. By IR, thermogravimetric and X-ray diffraction we establish the maximum degree of dye loading obtained (1.5 molecules per unit cell) and by modeling we reveal that at these conditions fluorenone molecules form quasi 1-D supramolecular nanoladders running along the zeolite channels. Spatial and morphological control provided by the nanoporous matrix combined with a complex blend of strong dye-zeolite and weaker dye-dye van der Walls interactions lie at the origin of this unique architecture, which is also stabilized by the hydrogen bond network of co-adsorbed water molecules surrounding the dye nanoladder and penetrating between its rungs.
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