ETH Zurich, Food & Soft Materials Science, Institute of Food, Nutrition, & Health, Schmelzbergstrasse 9, LFO, E 23, 8092 Zürich, Switzerland.
Langmuir. 2011 May 17;27(10):6171-8. doi: 10.1021/la200116e. Epub 2011 Apr 21.
We present comprehensive results on the microrheological study of lyotropic liquid crystalline phases of various space groups constituted by water-monoglyceride (Dimodan) mixtures. In order to explore the viscoelastic properties of these systems, we use particle tracking of probe colloidal particles suitably dispersed in the liquid crystals and monitored by diffusing wave spectroscopy. The identification of the various liquid crystalline phases was separately carried out by small-angle X-ray scattering. The restricted motion of the particles was monitored and identified by the decay time of intensity autocorrelation function and the corresponding time-dependent mean square displacement (MSD), which revealed space group-dependent behavior. The characteristic time extracted by the intersection of the slopes of the MSD at short and long time scales, provided a characteristic time which could be directly compared with the relaxation time obtained by microrheology. Further direct comparison of microrheology and bulk rheology measurements was gained via the Laplace transform of the generalized time-dependent MSD, yielding the microrheology storage and loss moduli, G'(ω) and G''(ω), in the frequency domain ω. The general picture emerging from the microrheology data is that all liquid crystals exhibit viscoelastic properties in line with results from bulk rheology and the transition regime (elastic to viscous) differs according to the specific liquid crystal considered. In the case of the lamellar phase, a plastic fluid is measured by bulk rheology, while microrheology indicates viscoelastic behavior. Although we generally find good qualitative agreement between the two techniques, all liquid crystalline systems are found to relax faster when studied with microrheology. The most plausible explanation for this difference is due to the different length scales probed by the two techniques: that is, microscopical relaxation on these structured fluids, is likely to occur at shorter time scales which are more suitably probed by microrheology, whereas bulk, macroscopic relaxations occurring at longer time scales can only be probed by bulk rheology.
我们展示了关于各向异性液晶相的微观流变学研究的综合结果,这些液晶相由水-单甘油脂(Dimodan)混合物组成。为了探索这些系统的粘弹性性质,我们使用适当分散在液晶中的探针胶体颗粒的粒子跟踪,并通过扩散波光谱进行监测。通过小角 X 射线散射分别确定了各种液晶相。通过强度自相关函数的衰减时间和相应的时均平方位移(MSD)来监测和识别颗粒的受限运动,这揭示了与空间群相关的行为。通过在短时间和长时间尺度上的 MSD 斜率的交点提取特征时间,可以得到一个可以直接与通过微观流变学获得的弛豫时间进行比较的特征时间。通过广义时变 MSD 的拉普拉斯变换进一步获得微观流变学和体流变学测量之间的直接比较,得到频域 ω 中的微观流变学储能和损耗模量 G'(ω)和 G''(ω)。从微观流变学数据中得出的总体情况是,所有液晶相都表现出与体流变学一致的粘弹性性质,并且弹性到粘性的转变区域根据所考虑的特定液晶相而不同。在层状相的情况下,体流变学测量到的是塑性流体,而微观流变学则表明存在粘弹性行为。尽管我们通常发现这两种技术之间存在良好的定性一致性,但当使用微观流变学进行研究时,所有液晶相的弛豫速度都更快。这种差异最可能的解释是由于两种技术探测的不同长度尺度:即这些结构化流体的微观弛豫可能在更适合微观流变学探测的较短时间尺度上发生,而在较长时间尺度上发生的体、宏观弛豫只能通过体流变学来探测。