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arXiv 0907.2329cond-mat.soft
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浓缩微凝胶体系中的多重动力学机制

Multiple dynamic regimes in concentrated microgel systems

David A. Sessoms, Irmgard Bischofberger, Luca Cipelletti, Véronique Trappe

摘要:

我们调查的动力学不均匀性在集体放松的浓缩微凝胶系统,其中的包装分数可以方便地通过改变温度而变化。填充分数依赖的机械性能的特征在于由流体-固体过渡,其中系统性能从粘性切换到弹性低频行为。从下面接近这种转变,我们发现动态中的空间相关性的范围增加。除了这个过渡,空间相关范围达到最大值,在整个可观察到的系统的大小约为5毫米。增加包装分数甚至进一步导致第二次过渡,其特征是发展的大区域的较低和较高的动态活动,以及彼此分离;相关范围在这一点上减少。空间相关长度对体积分数的这种显著的非单调依赖性使人想起最近在颗粒系统中的堵塞/刚性转变处观察到的行为(Lechenault等人,2008)。我们确定这第二个过渡到“压缩”状态的过渡,系统的组成部分开始施加直接的接触力在对方身上,这样的动态变得越来越确定不平衡的应力。这种转变的证据也被发现在频率依赖性的存储和损耗模量,这变得越来越多地耦合作为直接摩擦之间的颗粒开始有助于系统内的耗散损耗。据我们所知,我们的数据提供了第一个观察到的动力学异质性的质的变化,从纯粹的热驱动的动态切换到应力驱动。

英文摘要:

We investigate dynamical heterogeneities in the collective relaxation of a concentrated microgel system, for which the packing fraction can be conveniently varied by changing the temperature. The packing fraction dependent mechanical properties are characterised by a fluid-solid transition, where the system properties switch from a viscous to an elastic low-frequency behaviour. Approaching this transition from below, we find that the range of spatial correlations in the dynamics increases. Beyond this transition, the spatial correlation range reaches a maximum, extending over the entire observable system size of approximately 5 mm. Increasing the packing fraction even further leads to a second transition, which is characterised by the development of large zones of lower and higher dynamical activity that are well separated from each other; the range of correlation decreases at this point. This striking non-monotonic dependence of the spatial correlation length on volume fraction is reminiscent of the behaviour recently observed at the jamming/rigidity transition in granular systems (Lechenault et al. 2008). We identify this second transition as the transition to 'squeezed' states, where the constituents of the system start to exert direct contact forces on each other, such that the dynamics becomes increasingly determined by imbalanced stresses. Evidence of this transition is also found in the frequency dependence of the storage and loss moduli, which become increasingly coupled as direct friction between the particles starts to contribute to the dissipative losses within the system. To our knowledge, our data provide the first observation of a qualitative change in dynamical heterogeneity as the dynamics switch from purely thermally-driven to stress-driven.

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