Enhancement of mechanical properties of nanocellulose xerogels using TEMPO-oxidized fibers.

We report xerogels prepared from TEMPO-oxidized cellulose nanofiber (Ox-CNF) that have enhanced yield stresses and Young's Modulus (E) up to 15.4 MPa. The xerogels were highly porous (>95 %) and were measured by density determination, SEM, Brunauer-Emmet-Teller (BET) experiments, and microCT analysis.

Needle-induced cavitation: A method to probe the local mechanics of brain tissue.

Traditional mechanical characterization of extremely soft tissues is challenging given difficulty extracting tissue, satisfying geometric requirements, keeping tissues hydrated, and securing the tissue in an apparatus without slippage. The heterogeneous nature and structural complexity of brain tissues on small length scales makes it especially difficult to characterize. Needle-induced cavitation (NIC) is a technique that overcomes these issues and can mechanically characterize brain tissues at precise, micrometer-scale locations.

Anisotropic Hydrogel Microelectrodes for Intraspinal Neural Recordings in vivo.

Creating durable, motion-compliant neural interfaces is crucial for accessing dynamic tissues under in vivo conditions and linking neural activity with behaviors. Utilizing the self-alignment of nano-fillers in a polymeric matrix under repetitive tension, here, we introduce conductive carbon nanotubes with high aspect ratios into semi-crystalline polyvinyl alcohol hydrogels and create electrically anisotropic percolation pathways through cyclic stretching. The resulting anisotropic hydrogel fibers (diameter of 187 ± 13 µm) exhibit fatigue resistance (20,000 cycles at 20% strain) with a stretchability of 64.

Mesoscale polymer arrays: high aspect ratio surface structures and their digital reconstruction.

Inspired by adhesive bio-filamentous structure, such as bacterial pili, this work details the methods used to fabricate and characterize a surface-anchored array of thin, flexible and shape-responsive mesoscale polymer ribbons with a length-to-thickness aspect ratio of up to 100 000. The resulting structures exhibit geometrically complex and dynamic morphologies consistent with elastocapillary bending that experience an increase in curvature over hours of aging due to creep. We develop a computational image analysis framework to generate 3D reconstructions of these densely crowded geometries and extract quantitative descriptors to demonstrate morphological changes due to aging.

Fabricating mesoscale polymer ribbons with tunable mechanical properties evaporative deposition and dewetting.

Synthetic replication of the precise mesoscale control found in natural systems poses substantial experimental challenges due to the need for manipulation across multiple length scales (from nano- to millimeter). We address this challenge by using a 'flow coating' method to fabricate polymer ribbons with precisely tunable dimensions and mechanical properties. Overcoming barriers that previously limited the achievable range of properties with this method, we eliminate the need for substrate patterning and post-processing etching to facilitate the production of high aspect ratio, filament-like ribbons across a range of polymers-from glassy polystyrene to elastomeric poly(butadiene), as well as poly(butadiene--styrene).

Control of polymers' amorphous-crystalline transition enables miniaturization and multifunctional integration for hydrogel bioelectronics.

Soft bioelectronic devices exhibit motion-adaptive properties for neural interfaces to investigate complex neural circuits. Here, we develop a fabrication approach through the control of metamorphic polymers' amorphous-crystalline transition to miniaturize and integrate multiple components into hydrogel bioelectronics. We attain an about 80% diameter reduction in chemically cross-linked polyvinyl alcohol hydrogel fibers in a fully hydrated state.

Bottlebrush Networks: A Primer for Advanced Architectures.

Bottlebrush networks (BBNs) are an exciting new class of materials with interesting physical properties derived from their unique architecture. While great strides have been made in our fundamental understanding of bottlebrush polymers and networks, an interdisciplinary approach is necessary for the field to accelerate advancements. This review aims to act as a primer to BBN chemistry and physics for both new and current members of the community.

Silicone elastomers and the Persson-Brener adhesion model.

Many modern anti-icing and anti-fouling coatings rely on soft, low surface energy elastomeric materials such as polydimethylsiloxane for their functionality. While the low surface energy is desirable for reducing adhesion, very little work considers the larger contribution to adhesive failure caused by the viscoelastic nature of elastomers. Here we examine several different siloxane elastomers using a JKR adhesion test, which was operated over a range of different speeds and temperatures.

Mechanical Behavior of Hybrid Thin Films Fabricated by Sequential Infiltration Synthesis in Water-Rich Environment.

Sequential infiltration synthesis (SIS) is an emerging technique for fabricating hybrid organic-inorganic materials with nanoscale precision and controlled properties. Central to SIS implementation in applications such as membranes, sensors, and functional coatings is the mechanical properties of hybrid materials in water-rich environments. This work studies the nanocomposite morphology and its effect on the mechanical behavior of SIS-based hybrid thin films of AlO-PMMA under aqueous environments.

The Impact of Polymerization Chemistry on the Mechanical Properties of Poly(dimethylsiloxane) Bottlebrush Elastomers.

We compare the low-strain mechanical properties of bottlebrush elastomers (BBEs) synthesized using ring-opening metathesis and free radical polymerization. Through comparison of experimentally measured elastic moduli and those predicted by an ideal, affine model, we evaluate the efficiency of our networks in forming stress-supporting strands. This comparison allowed us to develop a structural efficiency ratio that facilitates the prediction of mechanical properties relative to polymerization chemistry (.

Adhesion and mechanical properties of poly(dimethylsiloxane) bottlebrush elastomers.

Poly(dimethylsiloxane) (PDMS) bottlebrush elastomers (BBEs) are attractive soft materials with well-controlled bulk mechanical properties. However, their surface and interfacial properties have not been studied in depth. We report a detailed study of the adhesion of PDMS BBEs to glass using a contact adhesion test to determine the critical energy release rates, , as a function of interfacial separation velocity.

Morphoelastic modelling of pattern development in the petal epidermal cell cuticle.

We use the model system as a vehicle to study the origin and propagation of surface nano-ridges in plant petal epidermal cells by tracking the development of the cell shape and the cuticle. In this system, the cuticle develops two distinct sub-layers, (i) an uppermost layer which increases in thickness and in-plane extension and (ii) a substrate, composed of cuticular and cell wall material. We quantify the pattern formation and geometrical changes and then postulate a mechanical model assuming that the cuticle behaves as a growing bi-layer.

Predicting the Electrical, Mechanical, and Geometric Contributions to Soft Electroadhesives through Fracture Mechanics.

Electroadhesion is the modulation of adhesive forces through electrostatic interactions and has potential applications in a number of next-generation technologies. Recent efforts have focused on using electroadhesion in soft robotics, haptics, and biointerfaces that often involve compliant materials and nonplanar geometries. Current models for electroadhesion provide limited insight on other contributions that are known to influence adhesion performance, such as geometry and material properties.

Control of Polymers' Amorphous-crystalline Transition for Hydrogel Bioelectronics Miniaturization and Multifunctional Integration.

Bioelectronic devices made of soft elastic materials exhibit motion-adaptive properties suitable for brain-machine interfaces and for investigating complex neural circuits. While two-dimensional microfabrication strategies enable miniaturizing devices to access delicate nerve structures, creating 3D architecture for expansive implementation requires more accessible and scalable manufacturing approaches. Here we present a fabrication strategy through the control of metamorphic polymers' amorphous-crystalline transition (COMPACT), for hydrogel bioelectronics with miniaturized fiber shape and multifunctional interrogation of neural circuits.

Structure-property relationships of velar bone tissue from the energy absorbing horncore of bighorn sheep rams.

Velar bone is the material that fills the horncore of bighorn sheep rams. The architectural dimensions of velar bone are orders of magnitude larger than trabecular bone, and velae are more sail-like compared to strut-like trabeculae. Velar bone is important for energy absorption and reduction of brain cavity accelerations during high energy head impacts, but velar bone material properties were previously unknown.

Self-spinning filaments for autonomously linked microfibers.

Filamentous bundles are ubiquitous in Nature, achieving highly adaptive functions and structural integrity from assembly of diverse mesoscale supramolecular elements. Engineering routes to synthetic, topologically integrated analogs demands precisely coordinated control of multiple filaments' shapes and positions, a major challenge when performed without complex machinery or labor-intensive processing. Here, we demonstrate a photocreasing design that encodes local curvature and twist into mesoscale polymer filaments, enabling their programmed transformation into target 3-dimensional geometries.

Interfacial cavitation.

Cavitation has long been recognized as a crucial predictor, or precursor, to the ultimate failure of various materials, ranging from ductile metals to soft and biological materials. Traditionally, cavitation in solids is defined as an unstable expansion of a void or a defect within a material. The critical applied load needed to trigger this instability -- the critical pressure -- is a lengthscale independent material property and has been predicted by numerous theoretical studies for a breadth of constitutive models.

Determining the elasto-adhesion length by void collapse in ultra-soft materials.

The elasto-adhesion length () is a materials property that describes the size scale where the relative importance of adhesion and elastic forces transitions for defined structures and functions. Conventional approaches for determining require independent measurements of the critical energy release rate () and Young's modulus (). Herein, we introduce a new method to obtain , only relying upon visual inspection.

Mesoscale Polymer Surfactants: Photolithographic Production and Localization at Droplet Interfaces.

Stabilization of fluid droplets, classically as oil-in-water or water-in-oil emulsions, is typically conducted using molecular surfactants or small particulates that localize at oil-water interfaces. In this paper, we describe a method whereby thin polymer films are converted photolithographically to ribbon-like mesoscale objects, which, in turn, adsorb to fluid interfaces where they extend as appendages, or arms, from the droplet surface. These "mesoscale polymer surfactants", or MPSs, were prepared from thin polymer films containing reactive functional moieties, including coumarin for photo-cross-linking, triphenylsulfonium for photoacid generation, and -butyl ester for solubility switching.

Geometry-controlled instabilities for soft-soft adhesive interfaces.

Soft materials interfaces can develop complex morphologies, such as cavities or finger-like features, during separation as a result of a mechanical instability. While the onset and growth of these instabilities have been investigated previously for interfaces between rigid and soft materials, no existing predictive model provides insight for controlling the separation morphology associated with these instabilities when both "sides" of the interface are soft. Here, we expand previous models to account for the geometry and materials properties of two soft materials that form an interface.

Shaping Nanoscale Ribbons into Microhelices of Controllable Radius and Pitch.

We report fabrication of highly flexible micron-sized helices from nanometer-thick ribbons. Building upon the helical coiling of such ultrathin ribbons mediated by surface tension, we demonstrate that the enhanced creep properties of highly confined materials can be leveraged to shape helices into the desired geometry with full control of the final shape. The helical radius, total length, and pitch angle are all freely and independently tunable within a wide range: radius within ∼1-100 μm, length within ∼100-3000 μm, and pitch angle within ∼0-70°.