Pathway-dependent supramolecular polymerization by planarity breaking

Veedu, Rasitha Manha; Fernández, Zulema; Bäumer, Nils; Albers, Antonia; Fernández, Gustavo

doi:10.1039/d4sc02499k

Chem. Sci.

2024

DOI: 10.1039/d4sc02499k

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Pathway-dependent supramolecular polymerization by planarity breaking

Rasitha Manha Veedu,

Zulema Fernández,

Nils Bäumer

et al.

Abstract: We introduce planarity breaking as a new design strategy for controlled supramolecular polymerization.

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Cited by 3 publications

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Pathway‐dependent Metallosupramolecular Polymerization Regulated by Ligand Geometry

Sutar,

Maisuls,

Fernández

et al. 2024

Chemistry A European J

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Understanding structure/property correlations in self‐assembly is a key but challenging requirement for developing functional materials. Herein, we explore the importance of ligand geometry to fine‐tune photophysical properties (MMLCT vs. MLCT excited states) and self‐assembly pathways in metallosupramolecular polymerization. To this end, we have designed two hydrophobic Pt(II) complexes, 1 and 2, containing a π‐extended bidentate bipyridine ligand with different substitution pattern, resulting in different molecular geometries (linear vs. V‐shaped). Detailed comparative studies revealed significant differences for both complexes in terms of their photophysical properties and self‐assembly pathways in non‐polar media. The V‐shaped topology of 1 enables facile face‐to‐face molecular stacking with a certain curvature leading to luminescent spherical assemblies exhibiting MMLCT states and short Pt⋅⋅⋅Pt contacts via a single‐step cooperative pathway. On the other hand, the higher preorganized linear topology of complex 2 induces a two‐step competitive self‐assembly process leading to the formation of one‐dimensional supramolecular polymers with slipped packing and MLCT‐originated emission. Our findings broaden the monomer scope for supramolecular polymerization and provide design guidelines for the realization of luminescent supramolecular assemblies.

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Pathway‐dependent Metallosupramolecular Polymerization Regulated by Ligand Geometry

Sutar,

Maisuls,

Fernández

et al. 2024

Chemistry A European J

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Self‐Assembly of Metallo‐Supramolecular Amphiphiles based on Azadipyrromethenes: Consecutive Pathways to Nanodiscs and Nanosheets

Zhang,

Hou,

Zhao

et al. 2024

Chemistry A European J

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A new class of metallo‐supramolecular amphiphilic dyes 1a, b was constructed by using two azadipyrromethene units which were respectively modified with two hydrophobic alkyl and two hydrophilic oligo(ethylene glycol) chains. The spectroscopic and morphological studies revealed the consecutive self‐assembly pathways of 1a in EtOH/H2O mixed solvent. The monomers of 1a firstly aggregated into the kinetic‐controlled, nanodisc‐shaped Agg. I upon cooling and the latter spontaneously transformed into the thermodynamically more stable Agg. II with a nanosheet morphology. While the non‐fluorescent Agg. I displayed a broad absorption band (λmax = 594 nm), the Agg. II displayed a more intensive and narrowed J‐band (λmax =693 nm) and a fluorescence band with a maximum at 760 nm (Фfl = 0.1), which could be ascribed to the J‐aggregation induced emission enhancement. The kinetics of Agg. I to Agg. II transformation was further modulated by seed‐initiated supramolecular polymerization with various ratios of Seedagg.II, in which the transformation rate was significantly increased by ca. 2 orders of magnitude compared to the spontaneous process. The supramolecular amphiphile 1b bearing longer hydrophilic chains formed only one type aggregate, which exhibited spectroscopic and morphological properties that were highly comparable with that of Agg. I.

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Impact of boron desymmetrization on supramolecular polymerization of BODIPY dyes

Tischer,

Fernández,

Borsdorf

et al. 2025

Org. Chem. Front.

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Pathway-dependent supramolecular polymerization by planarity breaking

Abstract: We introduce planarity breaking as a new design strategy for controlled supramolecular polymerization.

Cited by 3 publications

References 72 publications

Pathway‐dependent Metallosupramolecular Polymerization Regulated by Ligand Geometry

Pathway‐dependent Metallosupramolecular Polymerization Regulated by Ligand Geometry

Self‐Assembly of Metallo‐Supramolecular Amphiphiles based on Azadipyrromethenes: Consecutive Pathways to Nanodiscs and Nanosheets

Impact of boron desymmetrization on supramolecular polymerization of BODIPY dyes

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