Nonequilibrium Self-Organization of Lipids into Hierarchically Ordered and Compositionally Graded Cylindrical Smectics
Nonequilibrium Self-Organization of Lipids into Hierarchically Ordered and Compositionally Graded Cylindrical Smectics
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DOI：
10.1021/acs.langmuir.1c02576
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发表时间：
2022-01-12
期刊：
影响因子：
3.9
通讯作者：
Liedberg, Bo
中科院分区：
文献类型：
--
作者：
Ho, James C. S.;Su, Wan-Chih;Liedberg, Bo
当某些两亲物的干物质遇到水时，一种壮观的界面不稳定性随之而来：它导致形成称为髓鞘图形的指状管状突起的集合体，宽数十微米，长数十至数百微米，代表了一类新的非平衡高阶自组织。在这里，我们报告说，当不饱和脂质，胆固醇和鞘磷脂的相分离混合物水合时，所得髓鞘打破对称性，并将其组成自由度与延伸的髓鞘形态相结合：它们产生互补的、层间径向梯度的胆固醇浓度（和鞘磷脂）和不饱和脂质，这与平衡形态中的层间横向相分离形成鲜明对比。此外，分子特异性化学的相应梯度（即，通过甲基-β-环糊精的胆固醇提取和通过霍乱毒素的GM（1）结合）产生不寻常的形态，包括组成分级的囊泡和弯曲的管。我们建议，在信息处理的各个分子的水合特性的动力学差异，而消耗能量决定了这种新颖的行为进行水合的脂质混合物。
When a dry mass of certain amphiphiles encounters water, a spectacular interfacial instability ensues: It gives rise to the formation of ensembles of fingerlike tubular protrusions called myelin figures.tens of micrometers wide and tens to hundreds of micrometers long.representing a novel class of nonequilibrium higher-order self-organization. Here, we report that when phase-separating mixtures of unsaturated lipid, cholesterol, and sphingomyelin are hydrated, the resulting myelins break symmetry and couple their compositional degrees of freedom with the extended myelinic morphology: They produce complementary, interlamellar radial gradients of concentrations of cholesterol (and sphingomyelin) and unsaturated lipid, which stands in stark contrast to interlamellar, lateral phase separation in equilibrated morphologies. Furthermore, the corresponding gradients of molecule-specific chemistries (i.e., cholesterol extraction by methyl-beta-cyclodextrin and GM(1) binding by cholera toxin) produce unusual morphologies comprising compositionally graded vesicles and buckled tubes. We propose that kinetic differences in the information processing of hydration characteristics of individual molecules while expending energy dictate this novel behavior of lipid mixtures undergoing hydration.