Self-Wrinkling in Polyacrylamide Hydrogel Bilayers.

Swelling of a gel film attached to a soft substrate can induce surface instability, which results in the formation of highly ordered patterns such as wrinkles and folds. This phenomenon has been exploited to fabricate functional devices and rationalize morphogenesis. However, obtaining centimeter-scale patterns without immersing the film in a solvent remains challenging. Here, we show that wrinkles with wavelengths of up to a few centimeters can be spontaneously created during the open-air fabrication of film-substrate bilayers of polyacrylamide (PAAm) hydrogels. When the film of an aqueous pregel solution of acrylamide prepared on the PAAm hydrogel substrate undergoes open-air gelation, hexagonally packed dimples initially emerge on the surface, which later evolve into randomly oriented wrinkles. The formation of such self-organized patterns can be attributed to the surface instability resulting from autonomous water transport in the bilayer system during open-air fabrication. The temporal evolution of the patterns can be ascribed to an increase in overstress in the hydrogel film due to continued water uptake. The wrinkle wavelength can be controlled in the centimeter-scale range by adjusting the film thickness of the aqueous pregel solution. Our self-wrinkling method provides a simple mechanism for the generation of swelling-induced centimeter-scale wrinkles without requiring an external solvent, which is unachievable with conventional approaches.

Capillary-Induced Wrinkle-to-Fold Transitions Under Biaxial Compression.

Wrinkles in bilayer systems comprising a thin stiff film attached to a soft substrate can globally transition into folds under sufficiently large compression. This phenomenon has been extensively studied primarily using uniaxially compressed systems. However, inducing the wrinkle-to-fold transition at designated locations on a wrinkled surface under small biaxial compression remains a challenge. In this study, we describe a method for causing randomly oriented wrinkles to locally evolve into folds using water droplets. When a droplet comes into contact with the random wrinkles that have spontaneously formed upon film deposition owing to residual biaxial compressive strains, radially extended folds instantaneously emerge at the droplet boundary. Upon water evaporation, the wrinkles beneath the droplet also undergo a transition, leaving a fold network. By contrast, the surface regions distant from where the droplet was placed retain the wrinkle morphology. The folded areas can be controlled by adjusting the volume and number of droplets. These transitions are enabled by the capillary forces of water that help to increase the local compressive strains. This capillary-induced wrinkle-to-fold transition provides a simple mechanism to develop folds in selected locations on wrinkled surfaces of film-substrate systems subject to small biaxial compression, which is unachievable with conventional approaches.

Spontaneous formation of aligned DNA nanowires by capillarity-induced skin folding.

Although DNA nanowires have proven useful as a template for fabricating functional nanomaterials and a platform for genetic analysis, their widespread use is still hindered because of limited control over the size, geometry, and alignment of the nanowires. Here, we document the capillarity-induced folding of an initially wrinkled surface and present an approach to the spontaneous formation of aligned DNA nanowires using a template whose surface morphology dynamically changes in response to liquid. In particular, we exploit the familiar wrinkling phenomenon that results from compression of a thin skin on a soft substrate. Once a droplet of liquid solution containing DNA molecules is placed on the wrinkled surface, the liquid from the droplet enters certain wrinkled channels. The capillary forces deform wrinkles containing liquid into sharp folds, whereas the neighboring empty wrinkles are stretched out. In this way, we obtain a periodic array of folded channels that contain liquid solution with DNA molecules. Such an approach serves as a template for the fabrication of arrays of straight or wrinkled DNA nanowires, where their characteristic scales are robustly tunable with the physical properties of liquid and the mechanical and geometrical properties of the elastic system.

Ultrastructural characterization of surface-induced platelet activation on artificial materials by transmission electron microscopy.

Platelet adhesion is one of the most pivotal events of blood clotting for artificial surfaces. However, the mechanisms of surface-induced platelet activation have not been fully been elucidated or visualized so far. In this study, we attempted to observe the internal structures and adhesion interfaces of human platelets attached to artificial surfaces by transmission electron microscopy (TEM) during the platelet activation process. We prepared observation samples by a conventional embedding method using EPON 812 resin. The sectioning was sliced perpendicular to the a-platelet/material interface. Observation by TEM indicates that internal granules coalesce in the center of the platelet accompanied by pseudopodial growth in the early stage of platelet activation. Pseudopodia from a platelet attach to the material interface not along a plane but at a point. In addition, along with the process of platelet activation, the gap between the platelet membrane and the material surface at the interface disappeared and a-platelet/material adhesion became much tighter. In the fully activated platelet stage, the platelet becomes thinner and tightly adheres to the substrate. As a result of comparative observation of an adherent platelet on polycarbonate (PC) and on amorphous carbon (a-C:H), it was found that internal granules release was inhibited more remarkably on a-C:H coating rather than on PC. Despite numerous technical difficulties in preparing sectional samples, such a study might prove the essential mechanism of biomaterial-related thrombosis, and it might become possible to modify the surfaces of materials to minimize material-related thrombosis.