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Secondary nucleation is an emerging approach for synthesizing higher-order supramolecular polymers with exciting topologies. However, a detailed understanding of growth processes and the synthesis of homochiral superstructures is yet to be demonstrated. Here, we report the non-covalent synthesis of dendritic homochiral superstructures using NIR triimide dyes as building blocks via a secondary nucleation elongation process. Detailed analysis of kinetics and temporal evolution of morphology indicates that the formation of dendritic homochiral superstructures proceeds via growth on the surface and growth from the surface of the seeds. The combination of these two processes leads to the formation of elegant homochiral superstructures with a size of ~0.4 mm, having a superhelix at the center and helical fibres as branches. Moreover, these dendritic homochiral superstructures exhibit significantly high chiro-optical photoresponse with the magnitude of g reaching a value as high as 0.55 - 0.6. Thus, our results provide insights into the growth process of homochiral superstructures with dendritic topology, which can be critically important for the design and optimization of chiral-selective optoelectronic devices leveraging controlled self-assembly.
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http://dx.doi.org/10.1038/s41467-024-55107-y | DOI Listing |
ACS Nano
September 2025
College of Chemistry and Chemical Engineering, Key Laboratory of Catalytic Conversion and Clean Energy in Universities of Shandong Province, Qufu Normal University, Qufu, Shandong 273165, China.
The transformation of metal nanocluster (MNC)-based heterochiral assemblies into their homochiral analogues is a compelling goal inspired by the ubiquitous homochirality observed in living systems. Owing to the intricate factors governing nanomaterial chirality, the precise control of supramolecular chirality in MNCs remains rarely demonstrated. Herein, we demonstrated the coassembly behavior of AuNCs protected by 6-propyl-2-thiouracil (AuPRT) with chiral mandelic acid (MA), which revealed the formation of hybrid chiral superstructures of - and -helices in a single system.
View Article and Find Full Text PDFChemistry
August 2025
Department of Synthetic Chemistry and Biological Chemistry, Graduate School of Engineering, Kyoto University, Katsura, Nishikyo-ku, Kyoto, 615-8510, Japan.
Chiral self-sorting, including both narcissistic and social self-sorting, can generate homochiral and heterochiral supramolecular assemblies, respectively. However, achieving control over both pathways through molecular design remains challenging. Herein, we designed a series of macrocyclic pillar[5]arene derivatives with linear chains that thread into the cavities of adjacent molecules in the crystal, forming 1D superstructures.
View Article and Find Full Text PDFSci Adv
July 2025
Henan Key Laboratory of Crystalline Molecular Functional Materials, and College of Chemistry, Zhengzhou University, Zhengzhou 450001, China.
Construction of artificial microscale helical superstructures holds great significance for understanding hierarchical evolution of chiral architectures in nature. However, fabricating microscale helical superstructures from metal clusters remains mysterious and challenging. Here, we achieved hierarchically assembled helical bowties with micrometer scale via electrostatic interaction-driven co-assembly of chiral Au clusters and -1,4-cyclohexanediamine.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
May 2025
Key Laboratory of Colloid and Interface Chemistry of Ministry of Education School of Chemistry and Chemical Engineering, Shandong University, Jinan, 250100, People's Republic of China.
Expression of chirality at macroscopic scale through solution-processed bottom-up assembly is accompanied by the formation of complex superstructures. It undergoes complicated pathway including the hierarchical organization of molecular blocks in a spontaneous and ordered manner. Here we present a cyclodipeptide platform which delicately expresses chirality at the macroscopic level.
View Article and Find Full Text PDFJ Am Chem Soc
February 2025
Henan Key Laboratory of Crystalline Molecular Functional Materials, College of Chemistry, Zhengzhou University, Zhengzhou 450001, P. R. China.
Handedness-controllable macroscopic helices are needed for understanding the chirality transfer through scales and design of high-performance devices. Bottom-up self-assembly rarely affords macroscopic helical superstructures because of accumulating disorder that is difficult to avoid during hierarchical self-assembly. Here, we demonstrate that tetragold clusters can assemble into macroscopic helices at the centimeter scale.
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