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The hierarchical self‐assembly process opens up great potential for the construction of nanostructural superlattices. Precise regulation of self‐assembled superlattices, however, remains a challenge. Even when the primary molecules are precise, the supramolecular motifs (or secondary building blocks) can vary dramatically. In the present work, we propose the concept of unimolecular nanoparticles (UMNPs). The UMNPs act as the supramolecular motif and directly pack into the superlattices. A highly branched giant molecule is presented. We systematically explore its conformations and the superlattice of this giant molecule. Moreover, intriguing complex phases are discovered when blending this UMNP with other conventional giant molecules. These binary mixtures provide direct evidence to support our previously proposed self‐sorting process in the self‐assembly of "soft alloys". The concept of UMNPs offers a unique approach toward more precise regulation of self‐assembled superlattices in soft matter. [ABSTRACT FROM AUTHOR]

The selective removal and immobilization of uranyl ions from aqueous solutions is essential for the sustainable development of nuclear energy. Herein, a robust lanthanide‐organic framework material (IHEP‐24) is developed for simultaneous fluorescence sensing, selective adsorption, and photocatalytic reduction of uranium, integrating three different functions in one material. The confined space formed by the coordination assembly of viologen derivative ligands and metal‐oxygen clusters can act as precise recognition sites for uranyl, allowing IHEP‐24 to efficiently detect and capture uranyl ions. In addition, the presence of a viologen‐based radical ligand enables IHEP‐24 to a further photocatalytic reduction of the adsorbed uranyl to amorphous UO2. The mechanisms of adsorption and photocatalysis are revealed by batch experiments, photoelectrochemical characterizations, and theoretical calculations. This study provides a reference for the construction of robust multi‐functional MOF materials and also provides support for the deep removal and immobilization of radionuclides from aqueous solution. [ABSTRACT FROM AUTHOR]

The quasiperiodic structures in metal alloys have been known to depend on the existence of icosahedral order in the melt. Among different phases observed in intermetallics, decagonal quasicrystal (DQC) structures have been identified in many glass-forming alloys yet remain inaccessible in bulk-state condensed soft matters. Via annealing the mixture of two giant molecules, the binary system assemblies into an axial DQC superlattice, which is identified comprehensively with meso-atomic accuracy. Analysis indicates that the DQC superlattice is composed of mesoatoms with an unusually broad volume distribution. The interplays of submesoatomic (molecular) and mesoatomic (supramolecular) local packings are found to play a crucial role in not only the formation of the metastable DQC superlattice but also its transition to dodecagonal quasicrystal and Frank-Kasper σ superlattices., Competing Interests: The authors declare no competing interest., (Copyright © 2022 the Author(s). Published by PNAS.)