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Capillarity-driven transport in nanoporous solids is ubiquitous in nature andis of increasing importance for the functionality of modern liquid-infusedengineering materials. During imbibition, highly curved menisci are driven bynegative Laplace pressures of several hundred atmospheres, exerting an enormouscontractile load on an increasing portion of the porous matrix. Due to thechallenge of simultaneously monitoring imbibition and deformation with highspatial resolution, the resulting coupling of solid elasticity to liquidcapillarity has remained largely unexplored. Here, we study water imbibition inmesoporous silica using optical imaging, gravimetry, and high-resolutiondilatometry. In contrast to an expected Laplace pressure-induced contraction,we find a square-root-of-time expansion and an additional abrupt lengthincrease when the menisci reach the top surface. The final expansion is absentwhen we stop the imbibition front inside the porous medium in a dynamicimbibition-evaporation equilibrium, as is typical for water transport andtranspiration in plants. These peculiar deformation behaviors are validated bysingle-nanopore molecular dynamics simulations and described by a continuummodel that highlights the importance of expansive surface stresses at the porewalls (Bangham effect) and the buildup or release of contractile Laplacepressures as nanoscale menisci collectively advance, arrest, or disappear. Ourmodel predicts that these observations are valid not only for water imbibitionin silica, but for any imbibition process in nanopores, regardless of theliquid/solid combination. This also suggests that simple deformationmeasurements can be used to quantify surface stresses and Laplace pressures ortransport in a wide variety of natural and artificial porous media.

Deformation Dynamics of Nanopores upon Water Imbibition