How microscopic chirality is reflected in macroscopic scale to form various chiral shapes, such as straight helicoids and spiral ribbons, and how the degree of macroscopic chirality can be controlled are a focus of studies on the shape formation of many biomaterials and supramolecular systems. This article investigates both experimentally and theoretically how the chiral arrangement of liquid crystal mesogens in twist-nematic-elastomer films induces the formation of helicoids and spiral ribbons because of the coupling between the liquid crystalline order and the elasticity. It is also shown that the pitch of the formed ribbons can be tuned by temperature variation. The results of this study will facilitate the understanding of physics for the shape formation of chiral materials and the designing of new structures on basis of microscopic chirality.
Designed porosity in coordination materials often relies on highly ordered crystalline networks, which provide stability upon solvent removal. However, the requirement for crystallinity often impedes control of higher degrees of morphological versatility, or materials processing. Herein, we describe a supramolecular approach to the synthesis of amorphous polymer materials with controlled microporosity. The strategy entails the use of robust metal–organic polyhedra (MOPs) as porous monomers in the supramolecular polymerization reaction. Detailed analysis of the reaction mechanism of the MOPs with imidazole-based linkers revealed the polymerization to consist of three separate stages: nucleation, elongation, and cross-linking. By controlling the self-assembly pathways, we successfully tuned the resulting macroscopic form of the polymers, from spherical colloidal particles to colloidal gels with hierarchical porosity. The resulting materials display distinct microporous properties arising from the internal cavity of the MOPs. This synthetic approach could lead to the fabrication of soft, flexible materials with permanent porosity.