纳米多孔微流控限域中溶致相变的时空编程
Spatio-temporal programming of lyotropic phase transition in nanoporous microfluidic confinements
AI总结：
本研究以溶致色团液晶为模型，在纳米多孔微流控限域中通过PDMS表面选择性渗透驱动相变，结合润湿性、表体比等调控实现溶致相变的时空编程，并用于微载物输运，为生物材料组装提供新范式。
摘要：
简单分子自组装为复杂相可由物理约束驱动，例如纳米多孔表面的选择性分子吸附作用。尽管表面介导的组装在生命演化中具有重要意义，但分子富集与组装的物理途径一直被忽视。本研究以溶致色团液晶（lyotropic chromonic liquid crystal）作为模型生物材料，将其限域在纳米多孔微流控环境中，研究由纳米多孔基底驱动的分子组装过程。我们证明，纳米多孔聚二甲基硅氧烷（PDMS）表面因对水分子的选择性渗透，可在等温条件下驱动无序各向同性相转变为有序向列相，以及更高阶的柱状相。通过协同调控限域结构的润湿性、表体比和表面形貌，我们实现了对溶致相变高度的空间和时间控制编程。结合延时偏振成像、定量图像处理和一个简单数学模型，我们分析了这些相变过程，并构建了一幅主图，阐明了表面润湿性和通道几何结构在可编程溶致相变中的作用。PDMS本征的纳米多孔性和限域截面，加上施加的润湿性，共同调控N-M相变的速率；而微流控几何结构和嵌入的形貌则能在目标位置触发相变。我们利用N-M相变过程中出现的长程有序性，驱动嵌入微载物的弹性-平流输运，展示了由可调相变调控的粒子操控概念。我们的结果提出了一种可编程的材料组装物理途径，并为遗传组分、生物载物和最小合成细胞的组装提供了新范式。
英文摘要：
Self-assembly of simple molecules into complex phases can be driven by physical constraints, for instance, due to selective molecular uptake by nanoporous surfaces. Despite the significance of surface-mediated assembly in evolution of life, physical routes to molecular enrichment and assembly have remained overlooked. Here, using a lyotropic chromonic liquid crystal as model biological material, confined within nanoporous microfluidic environments, we study molecular assembly driven by nanoporous substrates. We demonstrate that nanoporous polydimethylsiloxane (PDMS) surfaces, due to selective permeation of water molecules, drive transition of disordered isotropic phase to ordered nematic, and higher order columnar phases under isothermal conditions. Synergistically, by tailoring the wettability, the surface-to-volume ratio, and surface topography of the confinements, we program the lyotropic phase transitions with a high degree of spatial and temporal control. Using a combination of timelapse polarized imaging, quantitative image processing, and a simple mathematical model, we analyze the phase transitions, and construct a master diagram capturing the role of surface wettability and channel geometry on programmable lyotropic phase transitions. Intrinsic PDMS nanoporosity and confinement cross-section, together with the imposed wettability regulate the rate of the N-M phase transition; whereas the microfluidic geometry and embedded topography enable phase transition at targeted locations. We harness the emergent long-range order during N-M transition to actuate elasto-advective transport of embedded micro-cargo, demonstrating particle manipulation concepts governed by tunable phase transitions. Our results present a programmable physical route to material assembly, and offer a new paradigm for assembling genetic components, biological cargo, and minimal synthetic cells.
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