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arXiv 1607.06367cond-mat.soft
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温度依赖的脂类非均匀转动关联

Temperature Dependent Heterogeneous Rotational Correlation in Lipids

Neda Dadashvand, Christina M. Othon

摘要:

脂质结构表现出复杂的和高度动态的横向结构;并且脂质密度和流动性的变化被认为在膜靶向和功能中起重要作用。液体在分子尺度上的动态结构可以表现出复杂的瞬态密度波动。在这里的横向异质性的脂质动力学探讨独立的脂质单层。随着温度的降低,探针表现出越来越广泛的和非均匀的旋转相关。这种异质性的增加似乎表现出临界起始,类似于玻璃形成流体中观察到的临界起始。我们通过测量荧光探针1-棕榈酰-2-[1]-sn-甘油-3-磷酸胆碱(NBD-PC)的旋转扩散,利用宽场时间分辨荧光各向异性(TRFA)研究了1,2-二肉豆蔻酰-sn-甘油-3-磷酸胆碱(DMPC)单组分脂质单层中的非均匀弛豫。所观察到的弛豫在高温(τ ~ 2.4 ns)下表现出窄的液体状分布,与之前的实验测量结果一致[1,2]。然而,随着温度的淬火,分布变宽,我们观察到一个长的弛豫人口(τ ~ 16.5 ns)的外观。这支持了在高堆积密度下观察到的脂质的异质性,并证明了脂质结构中的纳米级扩散和重组可以是显著复杂的,即使在最简单的无定形结构中。这种形式的动力学异质性可以对脂质膜结构的组织、渗透性和能量学产生显著影响。

英文摘要:

Lipid structures exhibit complex and highly dynamic lateral structure; and changes in lipid density and fluidity are believed to play an essential role in membrane targeting and function. The dynamic structure of liquids on the molecular scale can exhibit complex transient density fluctuations. Here the lateral heterogeneity of lipid dynamics is explored in free standing lipid monolayers. As the temperature is lowered the probes exhibit increasingly broad and heterogeneous rotational correlation. This increase in heterogeneity appears to exhibit a critical onset, similar to those observed for glass forming fluids. We explore heterogeneous relaxation in in a single constituent lipid monolayer of 1,2-dimyristoyl-sn-glycero-3-phosphocholine (DMPC) by measuring the rotational diffusion of a fluorescent probe, 1-palmitoyl-2-[1]-sn-glycero-3-phosphocholine (NBD-PC), using wide-field time-resolved fluorescence anisotropy (TRFA). The observed relaxation exhibits a narrow, liquid-like distribution at high temperatures (τ ~ 2.4 ns), consistent with previous experimental measures [1, 2]. However, as the temperature is quenched, the distribution broadens, and we observe the appearance of a long relaxation population (τ ~ 16.5 ns). This supports the heterogeneity observed for lipids at high packing densities, and demonstrates that the nanoscale diffusion and reorganization in lipid structures can be significantly complex, even in the simplest amorphous architectures. Dynamical heterogeneity of this form can have a significant impact on the organization, permeability and energetics of lipid membrane structures.

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