Rubber-like elasticity in laser-driven free surface flow of a Newtonian fluid

Abstract

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 𝜏M. For times considerably longer than 𝜏M 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, J. Mol. Struct. 972, 16–21 (2010), A. Zaccone, K. Trachenko, Proc. Natl. Acad. Sci. U.S.A. 117, 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 𝜏M. The dynamic shows that this persistence cannot originate from the far tail of a distribution of relaxation times around 𝜏M 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 10^6 s^(−1), 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.

Zhipeng Huang

Senior Research Associate

My research interests include ultrafast electron/X-ray diffraction, ultrafast spectroscopies, non-linear optics, (ultrafast) chemical and physical dynamics at surface or interface, etc.