论文标题

通过脂质囊泡的刺激反应性聚合物刷的可切换润湿:实验和仿真

Switchable Wetting of Stimulus Responsive Polymer Brushes by Lipid Vesicles: Experiments and Simulations

论文作者

Weissenfeld, Felix, Wesenberg, Lucia, Nakahata, Masaki, Müller, Marcus, Tanaka, Motomu

论文摘要

我们在平面脂质膜上定义的表面密度上嫁接了含有半胱氨酸侧链的聚丙烯酸刷。镜面X射线反射率数据表明,添加CD2+离子会诱导聚合物刷层的压实,并调节脂质囊泡的粘附。临界阈值水平诱导从非润湿到部分润湿状态的开关,[CD2+] = 0.25 mm,通过微介入测定法确定。囊泡和刷子之间的相互作用是通过与刷子接触的膜的高度波动以及表面附近的囊泡形状进行评估的。为了分析这些实验,我们研究了轴向对称囊泡的粘附,以通过模拟进行有限范围的膜 - 基底相互作用和浮力。我们发现,将粘附区边缘最大曲率与粘附强度相关的局部横向条件仍然相当准确。因此,尽管在实验上不可能以零浮力制备囊泡,但我们可以使用横向条件来估计粘附强度。然而,通过有限的膜 - 底物相互作用和浮力来显着修改粘附图。为了向下浮力,囊泡仅在底物上沉积,并且没有平均场粘附过渡。为了向上浮力,粘附的囊泡充其量是可稳定的。因此,仅在消失的浮力时才能发生平均场粘附过渡。仅对于零范围的膜 - 基底相互作用才能在有限的相互作用强度下发生二阶粘附过渡。对于任何有限范围的相互作用,当膜 - 底层相互作用从排斥力变为有吸引力时,发生过渡。我们提出了一个粘附图作为粘附强度和浮力的函数,并比较囊泡与液体液滴的润湿行为的粘附行为。

We grafted polyacrylic acid brushes containing cysteine side chains at a defined surface density on planar lipid membranes. Specular X-ray reflectivity data indicated that the addition of Cd2+ ions induces the compaction of the polymer brush layer and modulates the adhesion of lipid vesicles. The critical threshold level inducing the switch from non-wetting to partial wetting state, [Cd2+] = 0.25 mM, was determined by microinterferometry. The interactions between vesicles and brushes were evaluated by height fluctuations of the membrane in contact with brushes and the shape of vesicles near the surface. To analyze these experiments, we have studied adhesion of axially symmetric vesicles for finite-range membrane-substrate interaction and buoyancy through simulations. We found that the local transversality condition that relates the maximal curvature at the edge of the adhesion zone to the adhesion strength remains rather accurate. Thus, although it is not experimentally possible to prepare vesicles at zero buoyancy, we can use the transversality condition to estimate the adhesion strength. However, the adhesion diagram is significantly modified by a finite range of membrane-substrate interaction and buoyancy. For downward buoyancy, vesicles merely sediment onto the substrate and there is no mean-field adhesion transition. For upward buoyancy, adhered vesicles are metastable at best. Thus, a mean-field adhesion transition can only occur at vanishing buoyancy. Only for zero-range membrane-substrate interaction does a second-order adhesion transition occur at finite interaction strength. For any finite-range interaction, the transition occurs when the membrane-substrate interaction changes from repulsive to attractive. We present a adhesion diagram as a function of adhesion strength and buoyancy and compare the adhesion behavior of vesicles to the wetting behavior of droplets of liquids.

扫码加入交流群

加入微信交流群

微信交流群二维码

扫码加入学术交流群,获取更多资源