High-speed laser speckle imaging to unravel picoliter drop-on-demand to substrate interaction.

Understanding phenomena such as evaporation and imbibition of picoliter droplets into porous substrates is crucial in printing industry to achieve a higher printing quality and print speed. After printing, the residual pigment must remain fixed at the desired location on a substrate and be of a desired volume to yield a high resolution and vibrantly printed page that has become the expectation of modern printing technology. Current research entails not only chemical composition of the ink but also how this links to the dynamics and interactions that occur between the ink and the substrate at every stage of the printed spot formation, including evaporation, wetting, and imbibition. In this paper, we present an instrument that can print on-demand picoliter volume droplets of ink onto substrates and then immediately record on evolution of the resulting dynamics when these two materials interact. This high-speed laser speckle imaging (HS-LSI) technique has been developed to monitor nanometer displacement of the drying and imbibing ink droplet at a high frame rate, up to 20000 Hz, given the short timescales of these interactions. We present the design of the instrument, discuss the related challenges and the theory underlying the LSI technique, specifically how photons non-evasively probe opaque objects in a multiple scattering regime, and show how this technique can unravel the dynamics of drying and imbibition. We will finish giving a validation on the instrument and an example of its usage.

Syneresis of Colloidal Gels: Endogenous Stress and Interfacial Mobility Drive Compaction.

Colloidal gels may experience syneresis, an increase in volume fraction through expulsion of the continuous phase. This poroelastic process occurs when adhesion to the container is weak compared to endogenous stresses which develop during gelation. In this work, we measure the magnitude of syneresis, ΔV/V_{0}, for gels composed of solid, rubber, and liquid particles. Surprisingly, despite a constant thermoresponsive interparticle potential, gels composed of liquid and elastic particles synerese to a far greater extent. We conclude that this magnitude difference arises from contrasting modes of stress relaxation within the colloidal gel during syneresis either by bending or stretching of interparticle bonds.

Development of a multi-position indentation setup: Mapping soft and patternable heterogeneously crosslinked polymer networks.

We present the development of a multi-position indentation setup capable of spatially mapping mechanically heterogeneous materials. A detailed description of the indentation instrumentation is first provided, emphasizing force sensitivity, noise reduction, and signal fidelity. We first present indentation experiments on soft hydrogels that are submerged in water and show how the large contributions to the measured force due to the air-water surface tension can be avoided. The displacement field of the indented hydrogel is visualized using fluorescently coated microspheres embedded in the hydrogel, allowing simultaneous mapping of the stress and strain fields for a soft polymer network. We then fabricate a polymer network with patterned elasticity using halftone UV lithography and map the elastic modulus with the multi-position indentation instrument. The applied UV pattern is found back in the measured elastic modulus map, showing the capability of the multi-position indentation setup to map mechanically heterogeneous polymer networks.

Critical Casimir interactions between colloids around the critical point of binary solvents.

Critical Casimir interactions between colloidal particles arise from the confinement of fluctuations of a near-critical solvent in the liquid gap between closely-spaced particles. So far, the comparison of theoretical predictions and experimental measurements of critical Casimir forces (CCFs) has focused on the critical solvent composition, while it has been lacking for off-critical compositions. We address this issue by investigating CCFs between spherical colloidal particles around the critical point of a binary solvent through a combination of experiments, previous Ising Monte Carlo simulation results and field-theoretical methods. By measuring the correlation length of the near-critical solvent and the pair potentials of the particles in terms of radial distribution functions and by determining the second virial coefficient, we test in detail theoretical predictions. Our results indicate that the critical Casimir theory gives quantitative correct predictions for the interaction potential between particles in a near critical binary mixture if weak preferential adsorption of the particle surface is taken into account.

Water retention against drying with soft-particle suspensions in porous media.

Polymers suspended in granular packings have a significant impact on water retention, which is important for soil irrigation and the curing of building materials. Whereas the drying rate remains constant during a long period for pure water due to capillary flow providing liquid water to the evaporating surface, we show that it is not the case for a suspension made of soft polymeric particles called microgels: The drying rate decreases immediately and significantly. By measuring the spatial water saturation and concentration of suspended particles with magnetic resonance imaging, we can explain these original trends and model the process. In low-viscosity fluids, the accumulation of particles at the free surface induces a recession of the air-liquid interface. A simple model, assuming particle transport and accumulation below the sample free surface, is able to reproduce our observations without any fitting parameters. The high viscosity of the microgel suspension inhibits flow towards the free surface and a drying front appears. We show that water vapor diffusion over a defined and increasing length sets the drying rate. These results and model allow for better controlling the drying and water retention in granular porous materials.

Water transfer and crack regimes in nanocolloidal gels.

Direct observations of the surface and shape of model nanocolloidal gels associated with measurements of the spatial distribution of water content during drying show that air starts to significantly penetrate the sample when the material stops shrinking. We show that whether the material fractures or not during desiccation, as air penetrates the porous body, the water saturation decreases but remains almost homogeneous throughout the sample. This air invasion is at the origin of another type of fracture due to capillary effects; these results provide insight into the liquid dynamics at the nanoscale.