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                產品分類 PRODCT
                文章詳情

                Modular Molecular Self-Assembly for Diversified Chiroptical Systems

                日期:2022-05-25 08:07
                瀏覽次數:46
                摘要:Bottom-up multicomponent molecular self-assembly is an efficient approach to fabricate and manipulate chiral nanostructures and their chiroptical activities such as the Cotton effect and circular polarized luminescence (CPL). However, the integrated coassembly suffers from spontaneous and inherent systematic pathway complexity with low yield and poor fidelity. Consequently, a rational design of chiral self-assembled systems with more than two components remains a significant challenge
                Bottom-up multicomponent molecular self-assembly is an efficient approach
                to fabricate and manipulate chiral nanostructures and their chiroptical activi
                ties such as the Cotton effect and circular polarized luminescence (CPL).
                However, the integrated coassembly suffers from spontaneous and inherent
                systematic pathway complexity with low yield and poor fidelity. Consequently,
                a rational design of chiral self-assembled systems with more than two
                components remains a significant challenge. Herein, a modularized, ternary
                molecular self-assembly strategy that generates chiroptically active materials
                at diverse hierarchical levels is reported. N-Terminated aromatic amino acids
                appended with binding sites for charge transfer and multiple hydrogen bonds
                undergo the evolution of supramolecular chirality with unique handedness
                and luminescent color, generating abundant CPL emission with high lumines
                cence dissymmetry factor values in precisely controlled modalities. Ternary
                coassembly facilitates high-water-content hydrogel formation constituted by
                super-helical nanostructures, demonstrating a helix to toroid topological tran
                sition. This discovery would shed light on developing complicated multicom
                ponent systems in mimicking biological coassembly events.
                systems, thermodynamic equilibrium and
                non-equilibrium aggregates coexist, origi
                nated from on and off-pathways.[8] The
                systematic pathway complexity would be
                magnified dramatically in case of mul
                tiple constituent self-assembly supported
                by weak forces excluding metal–ligand
                coordination.[9,10] Two-component systems
                suffer from mixed coassembly and self
                sorting pathways, depending on the non
                covalent binding competition and other
                factors.[11,12] For a further consideration,
                there would be more than 20 possible
                pathways or combinations in a ternary
                system, and the number would rise to
                ≈200 for a quadruple component system.
                Although artificial multiple constituent
                systems (such as ternary and quadruple
                systems) possess advantages in synthe
                sizing soft materials with advanced pho
                tophysical properties in a more precise
                manner, such significant systematic com
                plexity brings along great challenges.[13–15]
                To overcome high systematic pathway complexity and fab
                ricate synergistically integrated soft materials that beyond two
                components, in this work, we employed two independent non
                covalent interactions including CT[16] and duplex hydrogen
                bonding interactions among N-terminated pyrene amino acids
                (namely PF and PV),[17] 1,3,5-tri(1H-benzo[d]imidazol-2-yl)
                benzene (TBIB) and 1,2,4,5-tetracyanobenzene (TCNB) for
                multicomponent molecular self-assembly (Figure 1). We estab
                lished a general principle that multi-constituent molecular self
                assembly could be modularized as different parts with distinct
                functions.[18–20] In this case, PF and PV (module A) are primary
                building blocks with chiral centers and binding sites to the other
                modules, where TBIB (module B) and TCNB (module C) could
                selectively bind to module A to allow for rational manipulation
                of modularized coassemblies via distinct attractive and repulsive
                forces. Molecular module ABC is not a mutual binding system,
                which has specific directional interactions upon noncovalent
                combination. Module A could bind to A, B, and C primarily via
                π–π stacking, duplex hydrogen bonding, and charge transfer
                (CT) interactions, generating functional chiroptical materials
                of AA, AB, and AC, respectively. However, due to the lack of
                sufficient weak interactions between TCNB and TBIB, the BC
                complexation is ruled out, avoiding unfavorable competitive
                pathways. For PV, it has the propensity to form ABC type ternary
                coassembly via duplex hydrogen bonding and CT interactions.
                The hierarchical integration allows for flexible synthesis
                of chiroptical materials with fine tailored Cotton effects,
                Q3
                Small 2020, 2002036
                UNCORREC

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