Self-emulsification, referring to the spontaneous formation of droplets of one phase in another immiscible phase, is attracting growing interest because of its simplicity in creating droplets. Existing self-emulsification methods usually rely on phase inversion, temperature cycling, and solvent evaporation. However, achieving spatiotemporal control over the morphology of self-emulsified droplets remains challenging. In this work, a conceptually new approach of creating both simple and complex droplets by self-emulsification of a phase-separating (SEPS) aqueous film, is reported. The aqueous film is formed by depositing a surfactant-laden aqueous droplet onto an aqueous surface, and the fragmentation of the film into droplets is triggered by a wetting transition. Smaller and more uniform droplets can be achieved by introducing liquid–liquid phase separation (LLPS). Moreover, properly modulating quadruple LLPS and film fragmentation enables the creation of highly multicellular droplets such as flower-like droplets stabilized by the interfacial self-assembly of nanoparticles. This work provides a novel strategy to design aqueous droplets by LLPS, and it will inspire a wide range of applications such as membraneless organelle synthesis, cell mimics and delivery.

中文翻译：

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通过相分离（SEPS）水膜的自乳化获得的花状液滴。

自乳化是指自发形成另一不混溶相中的一相液滴，由于其易于产生液滴，因此引起了越来越多的关注。现有的自乳化方法通常依赖于相转化，温度循环和溶剂蒸发。然而，实现对自乳化液滴的形态的时空控制仍然具有挑战性。在这项工作中，报告了通过相分离（SEPS）水膜的自乳化产生简单和复杂液滴的概念上新的方法。通过将载有表面活性剂的水性液滴沉积到水性表面上来形成水性膜，并且通过润湿转变来触发膜的分裂成液滴。通过引入液相-液相分离（LLPS），可以实现更小，更均匀的液滴。此外，适当调节四倍的LLPS和膜碎裂可以创建高度多细胞的液滴，例如通过纳米粒子的界面自组装而稳定的花朵状液滴。这项工作提供了一种通过LLPS设计水滴的新颖策略，它将激发广泛的应用，例如无膜细胞器合成，细胞模拟和递送。