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Item type:Publication, Access status: with files , Deformation dynamics of nanopores upon water imbibition(National Acad. of Sciences, 2024-09-17); ; ; ; Capillarity-driven transport in nanoporous solids is ubiquitous in nature and is of increasing importance for the functionality of modern liquid-infused engineering materials. During imbibition, highly curved menisci are driven by negative Laplace pressures of several hundred atmospheres, exerting an enormous contractile load on an increasing portion of the porous matrix. Due to the challenge of simultaneously monitoring imbibition and deformation with high spatial resolution, the resulting coupling of solid elasticity to liquid capillarity has remained largely unexplored. Here, we study water imbibition in mesoporous silica using optical imaging, gravimetry, and high-resolution dilatometry. In contrast to an expected Laplace pressure-induced contraction, we find a square-root-of-time expansion and an additional abrupt length increase when the menisci reach the top surface. The final expansion is absent when we stop the imbibition front inside the porous medium in a dynamic imbibition-evaporation equilibrium, as is typical for water transport and transpiration in plants. These peculiar deformation behaviors are validated by single-nanopore molecular dynamics simulations and described by a continuum model that highlights the importance of expansive surface stresses at the pore walls (Bangham effect) and the buildup or release of contractile Laplace pressures as nanoscale menisci collectively advance, arrest, or disappear. Our model predicts that these observations are valid not only for water imbibition in silica, but for any imbibition process in nanopores, regardless of the liquid/solid combination. This also suggests that simple deformation measurements can be used to quantify surface stresses and Laplace pressures or transport in a wide variety of natural and artificial porous media.Publicationtype: Journal Article75 49 - Some of the metrics are blocked by yourconsent settings
Item type:Publication, Access status: with files , Polymeric liquids in mesoporous photonic structures: from precursor film spreading to imbibition dynamics at the nanoscale(American Institute of Physics (AIP), 2024-02-14); ; ; ; Polymers are known to wet nanopores with high surface energy through an atomically thin precursor film followed by slower capillary filling. We present here light interference spectroscopy using a mesoporous membrane-based chip that allows us to observe the dynamics of these phenomena in situ down to the sub-nanometer scale at milli- to microsecond temporal resolution. The device consists of a mesoporous silicon film (average pore size 6 nm) with an integrated photonic crystal, which permits to simultaneously measure the phase shift of thin film interference and the resonance of the photonic crystal upon imbibition. For a styrene dimer, we find a flat fluid front without a precursor film, while the pentamer forms an expanding molecular thin film moving in front of the menisci of the capillary filling. These different behaviors are attributed to a significantly faster pore-surface diffusion compared to the imbibition dynamics for the pentamer and vice versa for the dimer. In addition, both oligomers exhibit anomalously slow imbibition dynamics, which could be explained by apparent viscosities of six and eleven times the bulk value, respectively. However, a more consistent description of the dynamics is achieved by a constriction model that emphasizes the increasing importance of local undulations in the pore radius with the molecular size and includes a sub-nanometer hydrodynamic dead, immobile zone at the pore wall but otherwise uses bulk fluid parameters. Overall, our study illustrates that interferometric, opto-fluidic experiments with mesoporous media allow for a remarkably detailed exploration of the nano-rheology of polymeric liquids.Publicationtype: Journal Article22 11 - Some of the metrics are blocked by yourconsent settings
Item type:Publication, Access status: with files , Laser-excited elastic guided waves reveal the complex mechanics of nanoporous silicon(Nature Publishing Group, 2021-06-14); ; ; ; Nanoporosity in silicon leads to completely new functionalities of this mainstream semiconductor. A difficult to assess mechanics has however significantly limited its application in fields ranging from nanofluidics and biosensorics to drug delivery, energy storage and photonics. Here, we present a study on laser-excited elastic guided waves detected contactless and non-destructively in dry and liquid-infused single-crystalline porous silicon. These experiments reveal that the self-organised formation of 100 billions of parallel nanopores per square centimetre cross section results in a nearly isotropic elasticity perpendicular to the pore axes and an 80% effective stiffness reduction, altogether leading to significant deviations from the cubic anisotropy observed in bulk silicon. Our thorough assessment of the wafer-scale mechanics of nanoporous silicon provides the base for predictive applications in robust on-chip devices and evidences that recent breakthroughs in laser ultrasonics open up entirely new frontiers for in-situ, non-destructive mechanical characterisation of dry and liquid-functionalised porous materials.Publicationtype: Journal ArticleScopus© Citations 25 149 326 - Some of the metrics are blocked by yourconsent settings
Item type:Publication, Access status: with files , Precursor film spreading during liquid imbibition in nanoporous photonic crystals(2020-12-01); ; ; ; When a macroscopic droplet spreads, a thin precursor film of liquid moves ahead of the advancing liquid-solid-vapor contact line. Whereas this phenomenon has been explored extensively for planar solid substrates, its presence in nanostructured geometries has barely been studied so far, despite its importance for many natural and technological fluid transport processes. Here we use porous photonic crystals in silicon to resolve by light interferometry capillarity-driven spreading of liquid fronts in pores of few nanometers in radius. Upon spatiotemporal rescaling the fluid profiles collapse on master curves indicating that all imbibition fronts follow a square-root-of-time broadening dynamics. For the simple liquid (glycerol) a sharp front with a widening typical of Lucas-Washburn capillary-rise dynamics in a medium with pore-size distribution occurs. By contrast, for a polymer (PDMS) a precursor film moving ahead of the main menisci entirely alters the nature of the nanoscale transport, in agreement with predictions of computer simulations.Publicationtype: Journal ArticleScopus© Citations 15 198 167