Anzivino Carmine, Xhani Klejdis, Carpineti Marina, Verrastro Stefano, Zaccone Alessio, Vailati Alberto
Department of Physics "A. Pontremoli", University of Milan, via Celoria 16, 20133 Milan, Italy.
J Phys Chem Lett. 2024 Sep 5;15(35):9030-9036. doi: 10.1021/acs.jpclett.4c01236. Epub 2024 Aug 27.
In a binary fluid mixture, the concentration gradient of a heavier molecular solute leads to a diffusive flux of solvent and solute to achieve thermodynamic equilibrium. If the solute concentration decreases with height, the system is always in a condition of stable mechanical equilibrium against gravity. We show experimentally that this mechanical equilibrium becomes unstable in case colloidal particles are dispersed uniformly within the mixture and that the resulting colloidal suspension undergoes a transient convective instability with the onset of convection patterns. By means of a numerical analysis, we clarify the microscopic mechanism from which the observed destabilization process originates. The solute concentration gradient drives an upward diffusiophoretic migration of colloids, in turn causing the development of a mechanically unstable layer within the sample, where the density of the suspension increases with height. Convective motions arise to minimize this localized rise in gravitational potential energy.
在二元流体混合物中,较重分子溶质的浓度梯度会导致溶剂和溶质的扩散通量,以实现热力学平衡。如果溶质浓度随高度降低,系统始终处于对抗重力的稳定机械平衡状态。我们通过实验表明,当胶体颗粒均匀分散在混合物中时,这种机械平衡会变得不稳定,并且由此产生的胶体悬浮液会随着对流模式的出现而经历瞬态对流不稳定性。通过数值分析,我们阐明了观察到的失稳过程所源自的微观机制。溶质浓度梯度驱动胶体向上进行扩散泳迁移,进而导致样品中形成一个机械不稳定层,在该层中悬浮液的密度随高度增加。对流运动的出现是为了使这种局部重力势能的增加最小化。