What question did this study set out to answer?

This research aims to explore the chiral amplification of supramolecular aggregates in aqueous environments and its implications for understanding homochirality.

May 20, 2026

Chiral Amplification in Dynamic Supramolecularly Tailored Aggregates with Enhanced Stimuli-Responsive Fluorescence Activity

Key Points

This research aims to explore the chiral amplification of supramolecular aggregates in aqueous environments and its implications for understanding homochirality.
Developed a concentration-dependent asymmetric hierarchical H-aggregate using PBM and β-CD.
Utilized techniques like UV–vis, PXRD, FT-IR, NMR, DLS, SEM, and AFM for analysis.
Applied light irradiation to observe transformations and measure fluorescence activity.
The 0.9 mM aqueous PBM@3β-CD solution showed a maximal intrinsic chirality expression of ∼50 folds.
Light irradiation converted it into a distorted J-aggregate while retaining chirality, with an effective coherence length (N ≈ 5).
The aggregation induced fluorescence featured a quantum yield of ΦF = 0.11 at 390 nm.

Abstract

Chiral amplification of supramolecular aggregates in a completely aqueous medium is a treasure trove to realize the origins of homochirality in nature. Here, we report the development of a concentration-dependent asymmetric hierarchical columnar H-aggregate from the repeated cooperative stacking of a propeller shaped complex between C3 symmetric protonated benzoylated melamine (PBM) and beta-cyclodextrin (β-CD) in water governed by π–π interaction and 3-fold H-bonding as evidenced by UV–vis, PXRD, FT-IR, 1D and 2D NMR, DLS, SEM, AFM, etc. Circular dichroism spectra demonstrated the overall intrinsic conformational chirality. A 0.9 mM aqueous solution of PBM@3β-CD exhibited the maximum expression of chirality (∼50 folds). Light irradiation has transformed it into distorted J-aggregate with retention of chirality with an effective coherence length (N ≈ 5). It showed brilliant aggregation induced fluorescence (AIF) with fluorescence quantum yield ΦF = 0.11 at 390 nm. The structure of the monomeric PBM@3β-CD was theoretically optimized. The expression of cooperativity from the synergistic interactions among the monomeric repeating units is elucidated by a nucleation-elongation model. Our results thus open new routes to understand multicomponent stimuli-responsive supramolecular host–guest self-assembly, offering valuable insights into the formed conformationally asymmetric superstructures.

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