The shape of Nature's stingers revealed.

Stinger-like structures in living organisms evolved convergently across taxa for both defensive and offensive purposes, with the main goal being penetration and damage. Our observations over a broad range of taxa and sizes, from microscopic radiolarians to narwhals, reveal a self-similar geometry of the stinger extremity: the diameter (d) increases along the distance from the tip (x) following a power law [Formula: see text] , with the tapering exponent varying universally between 2 and 3. We demonstrate, through analytical and experimental mechanics involving three-dimensional (3D) printing, that this geometry optimizes the stinger's performance; it represents a trade-off between the propensity to buckle, for n smaller than 2, and increased penetration force, for n greater than 3. Moreover, we find that this optimal tapering exponent does not depend on stinger size and aspect ratio (base diameter over length). We conclude that for Nature's stingers, composed of biological materials with moduli ranging from hundreds of megapascals to ten gigapascals, the necessity for a power-law contour increases with sharpness to ensure sufficient stability for penetration of skin-like tissues. Our results offer a solution to the puzzle underlying this universal geometric trait of biological stingers and may provide a new strategy to design needle-like structures for engineering or medical applications.

A bioinspired snap-through metastructure for manipulating micro-objects.

Micro-objects stick tenaciously to each other-a well-known show-stopper in microtechnology and in handling micro-objects. Inspired by the trigger plant, we explore a mechanical metastructure for overcoming adhesion involving a snap-action mechanism. We analyze the nonlinear mechanical response of curved beam architectures clamped by a tunable spring, incorporating mono- and bistable states. As a result, reversible miniaturized snap-through devices are successfully realized by micron-scale direct printing, and successful pick-and-place handling of a micro-object is demonstrated. The technique is applicable to universal scenarios, including dry and wet environment, or smooth and rough counter surfaces. With an unprecedented switching ratio (between high and low adhesion) exceeding 104, this concept proposes an efficient paradigm for handling and placing superlight objects.

Film-Terminated Fibrillar Microstructures with Improved Adhesion on Skin-like Surfaces.

Adhesives for interaction with human skin and tissues are needed for multiple applications. Micropatterned dry adhesives are potential candidates, allowing for a conformal contact and glue-free adhesion based on van der Waals interactions. In this study, we investigate the superior adhesion of film-terminated fibrillar microstructures (fibril diameter, 60 µm; aspect ratio, 3) in contact with surfaces of skin-like roughness (Rz 50 µm). Adhesion decays only moderately with increasing roughness, in contrast to unstructured samples. Sinusoidal model surfaces adhere when their wavelengths exceed about four fibril diameters. The film-terminated microstructure exhibits a saturation of the compressive force during application, implying a pressure safety regime protecting delicate counter surfaces. Applications of this novel adhesive concept are foreseen in the fields of wearable electronics and wound dressing.

Attachment of bioinspired microfibrils in fluids: transition from a hydrodynamic to hydrostatic mechanism.

Reversible and switchable adhesion of elastomeric microstructures has attracted significant interest in the development of grippers for object manipulation. Their applications, however, have often been limited to dry conditions and adhesion of such deformable microfibrils in the fluid environment is less understood. In the present study, we performed adhesion tests in silicone oil using single cylindrical microfibrils of a flat-punch shape with a radius of 80 µm. Stiff fibrils were created using three-dimensional printing of an elastomeric resin with an elastic modulus of 500 MPa, and soft fibrils, with a modulus of 3.3 MPa, were moulded in polyurethane. Our results suggest that adhesion is dominated by hydrodynamic forces, which can be maximized by stiff materials and high retraction velocities, in line with theoretical predictions. The maximum pull-off stress of stiff cylindrical fibrils is 0.6 MPa, limited by cavitation and viscous fingering, occurring at retraction velocities greater than 2 µm s-1. Next, we add a mushroom cap to the microfibrils, which, in the case of the softer material, deforms upon retraction and leads to a transition to a hydrostatic suction regime with higher pull-off stresses ranging from 0.7 to 0.9 MPa. The effects of elastic modulus, fibril size and viscosity for underwater applications are illustrated in a mechanism map to provide guidance for design optimization.

Water as a "glue": Elasticity-enhanced wet attachment of biomimetic microcup structures.

Octopus, clingfish, and larva use soft cups to attach to surfaces under water. Recently, various bioinspired cups have been engineered. However, the mechanisms of their attachment and detachment remain elusive. Using a novel microcup, fabricated by two-photon lithography, coupled with in situ pressure sensor and observation cameras, we reveal the detailed nature of its attachment/detachment under water. It involves elasticity-enhanced hydrodynamics generating "self-sealing" and high suction at the cup-substrate interface, converting water into "glue." Detachment is mediated by seal breaking. Three distinct mechanisms of breaking are identified, including elastic buckling of the cup rim. A mathematical model describes the interplay between the attachment/detachment process, geometry, elasto-hydrodynamics, and cup retraction speed. If the speed is too slow, then the octopus cannot attach; if the tide is too gentle for the larva, then water cannot serve as a glue. The concept of "water glue" can innovate underwater transport and manufacturing strategies.

Optoacoustically induced auditory brainstem responses in the mouse model enhanced through an absorbing film.

SIGNIFICANCE: Optoacoustic stimulation offers an alternative stimulation strategy for the hearing organ. To serve as the base for a novel auditory prosthesis, the optoacoustic stimulation must be biocompatible and energy-saving. AIM: Enhancing the efficiency of optoacoustic stimulation while reducing the energy input in a suited animal model. APPROACH: Optoacoustically induced auditory brainstem responses (oABRs) were recorded after the pulsed laser irradiation of the tympanic membrane (TM) in mice. The results were compared with the ABRs induced through acoustic click stimulation. In addition, self-adhesive absorbing films were applied on the TM before the optoacoustic stimulation to investigate their effect on the resulting ABRs. RESULTS: Using an absorbing film on the TM during optical stimulation led to considerably enhanced oABR wave I amplitude values compared with the stimulation of the bare TM. When using our stimulation strategy, we induced oABR waves in the 50% to 60% range of the acoustical stimulation reached with 80-dB SPL click stimuli. CONCLUSIONS: The mouse model can be used for certain developmental work for an optoacoustic auditory prosthesis. Using absorbing films on the TM during optical stimulation considerably enhances oABR wave I amplitude. Optimization of the stimulation strategy could further enhance the efficiency within biocompatibility margins.

Enhancing Dry Adhesion of Polymeric Micropatterns by Electric Fields.

Micropatterned dry adhesives rely mainly on van der Waals interactions. In this paper, we explore the adhesion strength increase that can be achieved by superimposing an electrostatic field through interdigitated subsurface electrodes. Micropatterns were produced by replica molding in silicone. The adhesion forces were characterized systematically by means of experiments and numerical modeling. The force increased with the square of the applied voltage for electric fields up to 800 V. For larger fields, a less-than-quadratic scaling was observed, which is likely due to the small, field-dependent electrical conductivity of the materials involved. The additional adhesion force was found to be up to twice of the field-free adhesion. The results suggest an alternative method for the controlled handling of fragile or miniaturized objects.

Statistical properties of defect-dependent detachment strength in bioinspired dry adhesives.

Dry adhesives using surface microstructures inspired by climbing animals have been recognized for their potentially novel capabilities, with relevance to a range of applications including pick-and-place handling. Past work has suggested that performance may be strongly dependent on variability in the critical defect size among fibrillar sub-contacts. However, it has not been directly verified that the resulting adhesive strength distribution is well described by the statistical theory of fracture used. Using in situ contact visualization, we characterize adhesive strength on a fibril-by-fibril basis for a synthetic fibrillar adhesive. Two distinct detachment mechanisms are observed. The fundamental, design-dependent mechanism involves defect propagation from within the contact. The secondary mechanism involves defect propagation from fabrication imperfections at the perimeter. The existence of two defect populations complicates characterization of the statistical properties. This is addressed by using the mean order ranking method to isolate the fundamental mechanism. The statistical properties obtained are subsequently used within a bimodal framework, allowing description of the secondary mechanism. Implications for performance are discussed, including the improvement of strength associated with elimination of fabrication imperfections. This statistical analysis of defect-dependent detachment represents a more complete approach to the characterization of fibrillar adhesives, offering new insight for design and fabrication.

Strong Wet and Dry Adhesion by Cupped Microstructures.

Recent advances in bio-inspired microfibrillar adhesives have resulted in technologies that allow reliable attachment to a variety of surfaces. Because capillary and van der Waals forces are considerably weakened underwater, fibrillar adhesives are however far less effective in wet environments. Although various strategies have been proposed to achieve strong reversible underwater adhesion, strong adhesives that work both in air and underwater without additional surface treatments have yet to be developed. In this study, we report a novel design-cupped microstructures (CM)-that generates strong controllable adhesion in air and underwater. We measured the adhesive performance of cupped polyurethane microstructures with three different cup angles (15, 30, and 45°) and the same cup diameter of 100 µm in dry and wet conditions in comparison to standard mushroom-shaped microstructures (MSMs) of the same dimensions. In air, 15°CM performed comparably to the flat MSM of the same size with an adhesion strength (force per real contact area) of up to 1.3 MPa, but underwater, 15°CM achieved 20 times stronger adhesion than MSM (∼1 MPa versus ∼0.05 MPa). Furthermore, the cupped microstructures exhibit self-sealing properties, whereby stronger pulls lead to longer stable attachment and much higher adhesion through the formation of a better seal.

A Self-Adhesive Elastomeric Wound Scaffold for Sensitive Adhesion to Tissue.

Pressure sensitive adhesives based on silicone materials are used particularly for skin adhesion, e.g., the fixation of electrocardiogram (ECG) electrodes or wound dressings. However, adhesion to sensitive tissue structures is not sufficiently addressed due to the risk of damage or rupture. We propose an approach in which a poly-(dimethylsiloxane) (PDMS)-based soft skin adhesive (SSA) acts as cellular scaffold for wound healing. Due to the intrinsically low surface free energy of silicone elastomers, functionalization strategies are needed to promote the attachment and spreading of eukaryotic cells. In the present work, the effect of physical adsorption of three different proteins on the adhesive properties of the soft skin adhesive was investigated. Fibronectin adsorption slightly affects adhesion but significantly improves the cellular interaction of L929 murine fibroblasts with the polymeric surface. Composite films were successfully attached to explanted tympanic membranes. This demonstrates the potential of protein functionalized SSA to act as an adhesive scaffold in delicate biomedical applications.

Thin Film Composite Silicon Elastomers for Cell Culture and Skin Applications: Manufacturing and Characterization.

In this protocol, we present methods to fabricate thin elastomer composite films for advanced cell culture applications and for the development of skin adhesives. Two different poly-(dimethyl siloxanes) (PDMS and soft skin adhesive (SSA)), have been used for in depth investigation of biological effects and adhesive characteristics. The composite films consist of a flexible backing layer and an adhesive top coating. Both layers have been manufactured by doctor blade application technique. In the present investigation, the adhesive behavior of the composite films has been investigated as a function of the layer thickness or a variation of the Young's modulus of the top layer. The Young's modulus of PDMS has been changed by varying the base to crosslinker mixing ratio. In addition, the thickness of SSA films has been varied from approx. 16 µm to approx. 320 µm. Scanning electron microscopy (SEM) and optical microscopy have been used for thickness measurements. The adhesive properties of elastomer films depend strongly on the film thickness, the Young's modulus of the polymers and surface characteristics. Therefore, normal adhesion of these films on glass substrates exhibiting smooth and rough surfaces has been investigated. Pull-off stress and work of separation are dependent on the mixing ratio of silicone elastomers. Additionally, the thickness of the soft skin adhesive placed on top of a supportive backing layer has been varied in order to produce patches for skin applications. Cytotoxicity, proliferation and cellular adhesion of L929 murine fibroblasts on PDMS films (mixing ratio 10:1) and SSA films (mixing ratio 50:50) have been conducted. We have shown here, for the first time, the side by side comparison of thin composite films manufactured of both polymers and present the investigation of their biological- and adhesive properties.

Adhesion and relaxation of a soft elastomer on surfaces with skin like roughness.

For designing new skin adhesives, the complex mechanical interaction of soft elastomers with surfaces of various roughnesses needs to be better understood. We systematically studied the effects of a wide set of roughness characteristics, film thickness, hold time and material relaxation on the adhesive behaviour of the silicone elastomer SSA 7-9800 (Dow Corning). As model surfaces, we used epoxy replicas obtained from substrates with roughness ranging from very smooth to skin-like. Our results demonstrate that films of thin and intermediate thickness (60 and 160 µm) adhered best to a sub-micron rough surface, with a pull-off stress of about 50 kPa. Significant variations in pull-off stress and detachment mechanism with roughness and hold time were found. In contrast, 320 µm thick films adhered with lower pull-off stress of about 17 kPa, but were less sensitive to roughness and hold time. It is demonstrated that the adhesion performance of the silicone films to rough surfaces can be tuned by tailoring the film thickness and contact time.

Roll-to-Roll Manufacturing of Micropatterned Adhesives by Template Compression.

For the next generation of handling systems, reversible adhesion enabled by micropatterned dry adhesives exhibits high potential. The versatility of polymeric micropatterns in handling objects made from various materials has been demonstrated by several groups. However, specimens reported in most studies have been restricted to the laboratory scale. Upscaling the size and quantity of micropatterned adhesives is the next step to enable successful technology transfer. Towards this aim, we introduce a continuous roll-to-roll replication process for fabrication of high-performance, mushroom-shaped micropatterned dry adhesives. The micropatterns were made from UV-curable polyurethane acrylates. To ensure the integrity of the complex structure during the fabrication process, flexible templates were used. The compression between the template and the wet prepolymer coating was investigated to optimize replication results without structural failures, and hence, to improve adhesion. As a result, we obtained micropatterned adhesive tapes, 10 cm in width and several meters in length, with adhesion strength about 250 kPa to glass, suitable for a wide range of applications.

Elevated temperature adhesion of bioinspired polymeric micropatterns to glass.

Micropatterned polymer surfaces that operate at various temperatures are required for emerging technical applications such as handling of objects or space debris. As the mechanical properties of polymers can vary significantly with temperature, adhesion performance can exhibit large variability. In the present paper, we experimentally study temperature effects on the adhesion of micropatterned adhesives (pillar length 20µm, aspect ratios 0.4 and 2) made from three different polymers, i.e., polydimethylsiloxane (PDMS), perfluoropolyether dimethacrylate (PFPEdma), and polyurethane (PU-ht). PU specimens showed the highest pull-off stresses of about 57kPa at 60°C, i.e., more than twice the value of unpatterned control samples. The work of separation similarly showed a maximum at that temperature, which was identified as the glass transition temperature, Tg. PDMS and PFPEdma specimens were tested above their Tg. As a result, the adhesion properties decreased monotonically (about 50% for both materials) for temperature elevation from 20 to 120°C. Overall, the results obtained in our study indicate that the operating temperature related to the glass transition temperature should be considered as a significant parameter for assessing the adhesion performance of micropatterned adhesives and in the technical design of adhesion devices.

Composite Pillars with a Tunable Interface for Adhesion to Rough Substrates.

The benefits of synthetic fibrillar dry adhesives for temporary and reversible attachment to hard objects with smooth surfaces have been successfully demonstrated in previous studies. However, surface roughness induces a dramatic reduction in pull-off stresses and necessarily requires revised design concepts. Toward this aim, we introduce cylindrical two-phase single pillars, which are composed of a mechanically stiff stalk and a soft tip layer. Adhesion to smooth and rough substrates is shown to exceed that of conventional pillar structures. The adhesion characteristics can be tuned by varying the thickness of the soft tip layer, the ratio of the Young's moduli and the curvature of the interface between the two phases. For rough substrates, adhesion values similar to those obtained on smooth substrates were achieved. Our concept of composite pillars overcomes current practical limitations caused by surface roughness and opens up fields of application where roughness is omnipresent.

Bioinspired polydimethylsiloxane-based composites with high shear resistance against wet tissue.

Patterned microstructures represent a potential approach for improving current wound closure strategies. Microstructures can be fabricated by multiple techniques including replica molding of soft polymer-based materials. However, polymeric microstructures often lack the required shear resistance with tissue needed for wound closure. In this work, scalable microstructures made from composites based on polydimethylsiloxane (PDMS) were explored to enhance the shear resistance with wet tissue. To achieve suitable mechanical properties, PDMS was reinforced by incorporation of polyethylene (PE) particles into the pre-polymer and by coating PE particle reinforced substrates with parylene. The reinforced microstructures showed a 6-fold enhancement, the coated structures even a 13-fold enhancement in Young׳s modulus over pure PDMS. Shear tests of mushroom-shaped microstructures (diameter 450µm, length 1mm) against chicken muscle tissue demonstrate first correlations that will be useful for future design of wound closure or stabilization implants.

Hierarchical macroscopic fibrillar adhesives: in situ study of buckling and adhesion mechanisms on wavy substrates.

Nature uses hierarchical fibrillar structures to mediate temporary adhesion to arbitrary substrates. Such structures provide high compliance such that the flat fibril tips can be better positioned with respect to asperities of a wavy rough substrate. We investigated the buckling and adhesion of hierarchically structured adhesives in contact with flat smooth, flat rough and wavy rough substrates. A macroscopic model for the structural adhesive was fabricated by molding polydimethylsiloxane into pillars of diameter in the range of 0.3-4.8 mm, with up to three different hierarchy levels. Both flat-ended and mushroom-shaped hierarchical samples buckled at preloads one quarter that of the single level structures. We explain this behavior by a change in the buckling mode; buckling leads to a loss of contact and diminishes adhesion. Our results indicate that hierarchical structures can have a strong influence on the degree of adhesion on both flat and wavy substrates. Strategies are discussed that achieve highly compliant substrates which adhere to rough substrates.

Temperature-Induced Switchable Adhesion using Nickel-Titanium-Polydimethylsiloxane Hybrid Surfaces.

A switchable dry adhesive based on a nickel-titanium (NiTi) shape-memory alloy with an adhesive silicone rubber surface has been developed. Although several studies investigate micropatterned, bioinspired adhesive surfaces, very few focus on reversible adhesion. The system here is based on the indentation-induced two-way shape-memory effect in NiTi alloys. NiTi is trained by mechanical deformation through indentation and grinding to elicit a temperature-induced switchable topography with protrusions at high temperature and a flat surface at low temperature. The trained surfaces are coated with either a smooth or a patterned adhesive polydimethylsiloxane (PDMS) layer, resulting in a temperature-induced switchable surface, used for dry adhesion. Adhesion tests show that the temperature-induced topographical change of the NiTi influences the adhesive performance of the hybrid system. For samples with a smooth PDMS layer the transition from flat to structured state reduces adhesion by 56%, and for samples with a micropatterned PDMS layer adhesion is switchable by nearly 100%. Both hybrid systems reveal strong reversibility related to the NiTi martensitic phase transformation, allowing repeated switching between an adhesive and a nonadhesive state. These effects have been discussed in terms of reversible changes in contact area and varying tilt angles of the pillars with respect to the substrate surface.

Nanostructured medical sutures with antibacterial properties.

Bacterial repellence in suture materials is a desirable property that can potentially improve the healing process by preventing infection. We describe a method for generating nanostructures at the surface of commercial sutures of different composition, and their potential for preventing biofilm formation. We show how bacteria attachment is altered in the presence of nanosized topographies and identify optimum designs for preventing it without compromising biocompatibility and applicability in terms of nanostructure robustness or tissue friction. These studies open new possibilities for flexible and cost-effective realization of topography-based antibacterial coatings for absorbable biomedical textiles.

Single macroscopic pillars as model system for bioinspired adhesives: influence of tip dimension, aspect ratio, and tilt angle.

The goal of our study is to better understand the design parameters of bioinspired dry adhesives inspired by geckos. For this, we fabricated single macroscopic pillars of 400 µm diameter with different aspect ratios and different tip shapes (i.e., flat tips, spherical tips with different radii, and mushroom tips with different diameters). Tilt-angle-dependent adhesion measurements showed that although the tip shape of the pillars strongly influences the pull-off force, the pull-off strength is similar for flat and mushroom-shaped tips. We found no tilt-angle dependency of adhesion for spherical tip structures and, except for high tilt angle and low preload experiments, no tilt-angle effect for mushroom-tip pillars. For flat-tip pillars, we found a strong influence of tilt angle on adhesion, which decreased linearly with increasing aspect ratio. The experiments show that for the tested aspect ratios between 1 and 5, a linear decrease of tilt-angle dependency is found. The results of our studies will help to design bioinspired adhesives for application on smooth and rough surfaces.