Spotted vesicles, striped micelles and Janus assemblies induced by ligand binding.
Spotted vesicles, striped micelles and Janus assemblies induced by ligand binding.
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多价两亲物混合物内多价配体的选择性结合原则上提供了一种驱动自组装结构域形成的机制。这里显示二价阳离子可交联聚阴离子两亲物，从而与中性两亲物分层并在囊泡内形成斑点或筏以及在圆柱形胶束内形成条纹。合成嵌段共聚物或天然脂质（PIP2、磷脂酰肌醇-4,5-二磷酸）的钙和铜交联结构域具有可调的尺寸、形状和/或间距，可以持续数年。这些“响应性 Janus 组件”中的横向偏析与曲率耦合较弱，并证明在相图中限制了 pH 值和阳离子浓度的狭窄区域，这些区域集中在多酸相互作用的特征结合常数附近。高 pH 下的重新混合令人惊讶，但强横向偏析 (SLS) 理论表明，反离子熵在静电交叉桥中占主导地位，从而说明了对自组装内配体诱导图案形成的见解。
Selective binding of multivalent ligands within a mixture of polyvalent amphiphiles provides, in principle, a mechanism to drive domain formation in self-assemblies. Divalent cations are shown here to crossbridge polyanionic amphiphiles that thereby demix from neutral amphiphiles and form spots or rafts within vesicles as well as stripes within cylindrical micelles. Calcium and copper crossbridged domains of synthetic block copolymers or natural lipid (PIP2, phosphatidylinositol-4,5-bisphosphate) possess tunable sizes, shapes, and/or spacings that can last for years. Lateral segregation in these ‘responsive Janus assemblies’ couples weakly to curvature and proves restricted within phase diagrams to narrow regimes of pH and cation concentration that are centered near the characteristic binding constants for polyacid interactions. Remixing at high pH is surprising, but a theory for Strong Lateral Segregation (SLS) shows that counterion entropy dominates electrostatic crossbridges, thus illustrating the insights gained into ligand induced pattern formation within self-assemblies.
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