Multiscale crack trapping for programmable adhesives.

The precise control of crack propagation at bonded interfaces is crucial for smart adhesives with advanced performance. However, previous studies have primarily concentrated on either microscale or macroscale crack propagation. Here, we present a hybrid adhesive that integrates microarchitectures and macroscopic nonlinear cut architectures for unparalleled adhesion control. The integration of these architectural elements enables conformal attachment and simultaneous crack trapping across multiple scales for high capacity, enhancing adhesion by more than 70×, while facilitating crack propagation at the macroscale in specific directions for programmable release and reusability. As adhesion strength and directionality can be independently controlled at any location, skin adhesive patches are created that are breathable, nondamaging, and exceptionally strong and secure yet remove easily. These capabilities are demonstrated with a skin-mounted adhesive patch with integrated electronics that accurately detects human motion and wirelessly transmits signals, enabling real-time control of avatars in virtual reality applications.

Enhancing Electrical Conductivity of Stretchable Liquid Metal-Silver Composites through Direct Ink Writing.

Structure-property-process relationships are a controlling factor in the performance of materials. This offers opportunities in emerging areas, such as stretchable conductors, to control process conditions during printing to enhance performance. Herein, by systematically tuning direct ink write (DIW) process parameters, the electrical conductivity of multiphase liquid metal (LM)-silver stretchable conductors is increased by a maximum of 400% to over 1.06 × 106 S·m-1. This is achieved by modulating the DIW print velocity, which enables the in situ elongation, coalescence, and percolation of these multiphase inclusions during printing. These DIW printed filaments are conductive as fabricated and are soft (modulus as low as 1.1 MPa), stretchable (strain limit >800%), and show strain invariant conductivity up to 80% strain. These capabilities are demonstrated through a set of electromagnetic induction coils that can transfer power wirelessly through air and water, even under deformation. This work provides a methodology to program properties in stretchable conductors, where the combination of material composition and process parameters leads to greatly enhanced performance. This approach can find use in applications such as soft robots, soft electronics, and printed materials for deformable, yet highly functional devices.

Kuttsukigami: sticky sheet design.

Shaping 3D objects from 2D sheets enables form and function in diverse areas from art to engineering. Here we introduce kuttsukigami, which exploits sheet-sheet adhesion to create structure. The technique allows thin sheets to be sculpted without requiring sharp folds, enabling structure in a broad range of materials for a versatile and reconfigurable thin-sheet engineering design scheme. Simple closed structures from cylindrical loops to complex shapes like the Möbius loop are constructed and modeled through the balance between deformation and adhesion. Importantly, the balance can be used to create experimental measurements of elasticity in complex morphologies. More practically, kuttsukigami is demonstrated to encapsulate objects from the kitchen to micro scales and to build on-demand logic gates through sticky electronic sheets for truly reusable, reconfigurable devices.

Metamaterial adhesives for programmable adhesion through reverse crack propagation.

Adhesives are typically either strong and permanent or reversible with limited strength. However, current strategies to create strong yet reversible adhesives needed for wearable devices, robotics and material disassembly lack independent control of strength and release, require complex fabrication or only work in specific conditions. Here we report metamaterial adhesives that simultaneously achieve strong and releasable adhesion with spatially selectable adhesion strength through programmed cut architectures. Nonlinear cuts uniquely suppress crack propagation by forcing cracks to propagate backwards for 60× enhancement in adhesion, while allowing crack growth in the opposite direction for easy release and reusability. This mechanism functions in numerous adhesives on diverse substrates in wet and dry conditions and enables highly tunable adhesion with independently programmable adhesion strength in two directions simultaneously at any location. We create these multifunctional materials in a maskless, digital fabrication framework to rapidly customize adhesive characteristics with deterministic control for next-generation adhesives.

X-ray scattering as an effective tool for characterizing liquid metal composite morphology.

Quantitative analysis of particle size and size distribution is crucial in establishing structure-property relationships of composite materials. An emerging soft composite architecture involves dispersing droplets of liquid metal throughout an elastomer, enabling synergistic properties of metals and soft polymers. The structure of these materials is typically characterized through real-space microscopy and image analysis; however, these techniques rely on magnified images that may not represent the global-averaged size and distribution of the droplets. In this study, we utilize ultra-small angle X-ray scattering (USAXS) as a reciprocal-space characterization technique that yields global-averaged dimensions of eutectic gallium indium (EGaIn) alloy soft composites. The Unified fit and Monte Carlo scattering methods are applied to determine the particle size and size distributions of the liquid metal droplets in the composites and are shown to be in excellent agreement with results from real-space image analysis. Additionally, all methods indicate that the droplets are getting larger as they are introduced into composites, suggesting that the droplets are agglomerating or possibly coalescing during dispersion. This work demonstrates the viability of X-ray scattering to elucidate structural information about liquid metal droplets for material development for applications in soft robotics, soft electronics, and multifunctional materials.

Tough Bonding of Liquid Metal-Elastomer Composites for Multifunctional Adhesives.

Liquid metal (LM) composites, which consist of LM droplets dispersed in highly deformable elastomers, have recently gained interest as a multifunctional material for soft robotics and electronics. The incorporation of LM into elastic solids allows for unique combinations of material properties such as high stretchability with thermal and electrical conductivity comparable to metals. However, it is currently a challenge to incorporate LM composites into integrated systems consisting of diverse materials and components due to a lack of adhesion control. Here, a chemical anchoring methodology to increase adhesion of LM composites to diverse substrates is presented. The fracture energy increases up to 100× relative to untreated surfaces, with values reaching up to 7800 J m-2 . Furthermore, the fracture energy, tensile modulus, and thermal conductivity can be tuned together by controlling the microstructure of LM composites. Finally, the bonding technique is used to integrate LM composites with functional electronic components without encapsulation or clamping, allowing for extreme deformations while maintaining exceptional thermal and electrical conductivity. These findings can accelerate the adoption of LM composites into complex soft robotic and electronic systems where strong, reliable bonding between diverse materials and components is required.

Octopus-inspired adhesive skins for intelligent and rapidly switchable underwater adhesion.

The octopus couples controllable adhesives with intricately embedded sensing, processing, and control to manipulate underwater objects. Current synthetic adhesive-based manipulators are typically manually operated without sensing or control and can be slow to activate and release adhesion, which limits system-level manipulation. Here, we couple switchable, octopus-inspired adhesives with embedded sensing, processing, and control for robust underwater manipulation. Adhesion strength is switched over 450× from the ON to OFF state in <50 ms over many cycles with an actively controlled membrane. Systematic design of adhesive geometry enables adherence to nonideal surfaces with low preload and independent control of adhesive strength and adhesive toughness for strong and reliable attachment and easy release. Our bio-inspired nervous system detects objects and autonomously triggers the switchable adhesives. This is implemented into a wearable glove where an array of adhesives and sensors creates a biomimetic adhesive skin to manipulate diverse underwater objects.

On-Demand Programming of Liquid Metal-Composite Microstructures through Direct Ink Write 3D Printing.

Soft, elastically deformable composites with liquid metal (LM) droplets can enable new generations of soft electronics, robotics, and reconfigurable structures. However, techniques to control local composite microstructure, which ultimately governs material properties and performance, is lacking. Here a direct ink writing technique is developed to program the LM microstructure (i.e., shape, orientation, and connectivity) on demand throughout elastomer composites. In contrast to inks with rigid particles that have fixed shape and size, it is shown that emulsion inks with LM fillers enable in situ control of microstructure. This enables filaments, films, and 3D structures with unique LM microstructures that are generated on demand and locked in during printing. This includes smooth and discrete transitions from spherical to needle-like droplets, curvilinear microstructures, geometrically complex embedded inclusion patterns, and connected LM networks. The printed materials are soft (modulus < 200 kPa), highly deformable (>600 % strain), and can be made locally insulating or electrically conductive using a single ink by controlling the process conditions. These capabilities are demonstrated by embedding elongated LM droplets in a soft heat sink, which rapidly dissipates heat from high-power LEDs. These programmable microstructures can enable new composite paradigms for emerging technologies that demand mechanical compliance with multifunctional response.

Shape morphing mechanical metamaterials through reversible plasticity.

Biological organisms such as the octopus can reconfigure their shape and properties to perform diverse tasks. However, soft machines struggle to achieve complex configurations, morph into shape to support loads, and go between multiple states reversibly. Here, we introduce a multifunctional shape-morphing material with reversible and rapid polymorphic reconfigurability. We couple elastomeric kirigami with an unconventional reversible plasticity mechanism in metal alloys to rapidly (<0.1 seconds) morph flat sheets into complex, load-bearing shapes, with reversibility and self-healing through phase change. This kirigami composite overcomes trade-offs in deformability and load-bearing capacity and eliminates power requirements to sustain reconfigured shapes. We demonstrate this material through integration with onboard control, motors, and power to create a soft robotic morphing drone, which autonomously transforms from a ground to air vehicle and an underwater morphing machine, which can be reversibly deployed to collect cargo.

Cancer cell migration in collagen-hyaluronan composite extracellular matrices.

Hyaluronan (HA) is a key component in the tumor microenvironment (TME) that participates in cancer growth and invasiveness. While the molecular weight (MW) dependent properties of HA can cause tumor-promoting and -repressing effects, the elevated levels of HA in the TME impedes drug delivery. The degradation of HA using hyaluronidases (HYALs), resulting in fragments of HA, is a way to overcome this, but the consequences of changes in HA molecular weight and concentration is currently unknown. Therefore, it is critical to understand the MW-dependent biological effects of HA. Here we examine the influence of HA molecular weight on biophysical properties that regulate cell migration and extracellular matrix (ECM) remodeling. In our study, we used vLMW, LMW and HMW HA at different physiologically relevant concentrations, with a particular interest in correlating the mechanical and structural properties to different cell functions. The elastic modulus, collagen network pore size and collagen fiber diameter increased with increasing HA concentration. Although the collagen network pore size increased, these pores were filled with the bulky HA molecules. Consequently, cell migration decreased with increase in HA concentration due to multiple, long-lived and unproductive protrusions, suggesting the influence of steric factors. Surprisingly, even though elastic modulus increased with HA molecular weight and concentration, gel compaction assays showed an increased degree of ECM compaction among HMW HA gels at high concentrations (2 and 4 mg mL-1 [0.2 and 0.4%]). These results were not seen in collagen gels that lacked HA, but had similar stiffness. HA appears to have the effect of decreasing migration and increasing collagen network contraction, but only at high HA molecular weight. Consequently, changes in HA molecular weight can have relatively large effects on cancer cell behavior. STATEMENT OF SIGNIFICANCE: Hyaluronan (HA) is a critical component of the tumor microenvironment (TME). Overproduction of HA in the TME results in poor prognosis and collapse of blood vessels, inhibiting drug delivery. Hyaluronidases have been used to enhance drug delivery. However, they lead to low molecular weight (MW) HA, altering the mechanical and structural properties of the TME and cancer cell behavior. Understanding how HA degradation affects cancer cell behavior is critical for uncovering detrimental effects of this therapy. Very little is known about how HA MW affects cancer cell behavior in tumor-mimicking collagen-HA composite networks. Here we examine how MW and HA content in collagen-HA networks alter structural and mechanical properties to regulate cell migration and matrix remodeling in 3D TME-mimicking environments.