Max Planck Institute for the Structure and Dynamics of Matter, 22761 Hamburg, Germany.
Proc Natl Acad Sci U S A. 2023 Jul 4;120(27):e2301956120. doi: 10.1073/pnas.2301956120. Epub 2023 Jun 26.
The energy needed to deform an elastic solid may be recovered, while in Newtonian fluids, like water and glycerol, deformation energy dissipates on timescales of the intermolecular relaxation time [Formula: see text] . For times considerably longer than [Formula: see text] the existence of shear elasticity requires long-range correlations, which challenge our understanding of the liquid state. We investigated laser-driven free surface bubbles in liquid glycerol by analyzing their expansion and bursting dynamics, in which we found a flow-dominating, rubber-like elasticity unrelated to surface tension forces. In extension to findings of a measurable liquid elasticity at even very low deformation frequencies [L. Noirez, P. Baroni, , 16-21 (2010), A. Zaccone, K. Trachenko, , 19653-19655 (2020)], that is difficult to access under increased strain, we find a robust, strain rate driven elasticity. The recovery of deformation energy allows the bursting bubble to reach Taylor-Culick velocities 20-fold higher than expected. The elasticity is persistent for microseconds, hence four orders of magnitude longer than [Formula: see text] . The dynamic shows that this persistence cannot originate from the far tail of a distribution of relaxation times around [Formula: see text] but must appear by frustrating the short molecular dissipation. The longer time should be interpreted as a relaxation of collective modes of metastable groups of molecules. With strain rates of 10 s, we observe a metastable glycerol shell exhibiting a rubber-like solid behavior with similar elasticity values and characteristic tolerance toward large strains, although the molecular interaction is fundamentally different.
弹性固体变形所需的能量可以恢复,而在牛顿流体(如水和甘油)中,变形能会在分子松弛时间 [Formula: see text] 的时间尺度上耗散。对于远大于 [Formula: see text] 的时间,剪切弹性的存在需要长程相关性,这挑战了我们对液态的理解。我们通过分析液态甘油中激光驱动的自由表面气泡的膨胀和破裂动力学来研究它们,在这个过程中我们发现了一种主导流动的、与表面张力无关的橡胶状弹性。除了在非常低的变形频率下可测量的液体弹性的发现[L. Noirez, P. Baroni, , 16-21 (2010), A. Zaccone, K. Trachenko, , 19653-19655 (2020)]之外,在应变增加的情况下很难获得这种弹性,我们还发现了一种稳健的、应变率驱动的弹性。变形能的恢复使得破裂气泡能够达到比预期高 20 倍的泰勒-库里克速度。这种弹性可以持续微秒,因此比 [Formula: see text] 长四个数量级。这种动态表明,这种持续时间不能源自围绕 [Formula: see text] 的松弛时间分布的长尾,而必须通过阻碍短分子耗散来产生。较长的时间应该被解释为亚稳分子团的集体模式的弛豫。在应变率为 10 s 的情况下,我们观察到一种亚稳甘油壳,它表现出类似于橡胶的固体行为,具有类似的弹性值和对大应变的特征容忍度,尽管分子相互作用在根本上是不同的。