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Abstract Adhesives that excel in wet or underwater environments are critical for applications ranging from healthcare and underwater robotics to infrastructure repair. However, achieving strong attachment and controlled release on difficult substrates, such as those that are curved, rough, or located in diverse fluid environments, remains a major challenge. Here, an octopus‐inspired adhesive with strong attachment and rapid release in challenging underwater environments is presented. Inspired by the octopus's infundibulum structure, a compliant, curved stalk, and an active deformable membrane for multi‐surface adhesion are utilized. The stalk's curved shape enhances conformal contact on large‐scale curvatures and increases contact stress for adaptability to small‐scale roughness. These synergistic mechanisms improve contact across multiple length scales, resulting in switching ratios of over 1000 within ≈30 ms with consistent attachment strength of over 60 kPa on diverse surfaces and conditions. These adhesives are demonstrated through the robust attachment and precise manipulation of rough underwater objects.more » « less
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Abstract Electrical and mechanical integration approaches are essential for emerging hybrid electronics that must robustly bond rigid electrical components with flexible circuits and substrates. However, flexible polymeric substrates and circuits cannot withstand the high temperatures used in traditional electronic processing. This constraint requires new strategies to create flexible materials that simultaneously achieve high electrical conductivity, strong adhesion, and processibility at low temperature. Here, an electrically conductive adhesive is introduced that is flexible, electrically conductive (up to 3.25×105S m−1) without sintering or high temperature post‐processing, and strongly adhesive to various materials common to flexible and stretchable circuits (fracture energy 350 <Gc< 700 J m−2). This is achieved through a multiphase soft composite consisting of an elastomeric and adhesive epoxy network with dispersed liquid metal droplets that are bridged by silver flakes, which form a flexible and conductive percolated network. These inks can be processed through masked deposition and direct ink writing at room temperature. This enables soft conductive wiring and robust integration of rigid components onto flexible substrates to create hybrid electronics for emerging applications in soft electronics, soft robotics, and multifunctional systems.more » « less
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Abstract Conductive adhesives are required for the integration of dissimilar material components to create soft electronic and robotic systems. Here, a heterogeneous liquid metal‐based conductive adhesive is developed that reversibly attaches to diverse surfaces with high stretchability (>100% strain), low modulus (<100 kPa), and strain‐invariant electrical conductivity. This SofT integrated composite with tacK through liquid metal (STICK‐LM) adhesive consists of a heterogeneous graded film with a liquid metal‐rich side that is embossed at prescribed locations for electrical conductivity and an electrically insulating adhesive side for integration. Adhesion behavior is tuned for adhesion energies > 70 Jm−2(≈ 25x enhancement over unmodified composites) and described with a viscoelastic analysis, providing design guidelines for controllable yet reversible adhesion in electrically conductive systems. The architecture of STICK‐LM adhesives provides anisotropic and heterogeneous electrical conductivity and enables direct integration into soft functional systems. This is demonstrated with deformable fuses for robotic joints, repositionable electronics that rapidly attach on curvilinear surfaces, and stretchable adhesive conductors with nearly constant electrical resistance. This study provides a methodology for electrically conductive, reversible adhesives for electrical and mechanical integration of multicomponent systems in emerging technologies.more » « less
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On‐Demand Programming of Liquid Metal‐Composite Microstructures through Direct Ink Write 3D PrintingAbstract 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.more » « less
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Abstract Rapidly controlling and switching adhesion is necessary for applications in robotic gripping and locomotion, pick and place operations, and transfer printing. However, switchable adhesives often display a binary response (on or off) with a narrow adhesion range, lack post‐fabrication adhesion tunability, or switch slowly due to diffusion‐controlled processes. Here, pneumatically controlled shape and rigidity tuning is coupled to rapidly switch adhesion (≈0.1 s) across a wide range of programmable adhesion forces with measured switching ratios as high as 1300x. The switchable adhesion system introduces an active polydimethylsiloxane membrane supported on a compliant, foam foundation with pressure‐tunable rigidity where positive and negative pneumatic pressure synergistically control contact stiffness and geometry to activate and release adhesion. Energy‐based modeling and finite element computation demonstrate that high adhesion is achieved through a pressure‐dependent, nonlinear stiffness of the foundation, while an inflated shape at positive pressures enables easy release. This approach enables adhesion‐based gripping and material assembly, which is utilized to pick‐and‐release common objects, rough and porous materials, and arrays of elements with a greater than 14 000xrange in mass. The robust assembly of diverse components (rigid, soft, flexible) is then demonstrated to create a soft and stretchable electronic device.more » « less
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Abstract A passive resonant sensor with kirigami patterning is presented to wirelessly report material deformation in closed systems. The sensors are fabricated from copper‐coated polyimide by etching a conductive Archimedean spiral and then laser cutting kirigami patterns. The sensor response is defined as the resonant frequency in the transmission scattering parameter signal (S21), which is captured via a benchtop vector network analyzer. The sensors are tested over a 0–22 cm range of extension and show a significant shift in resonant frequency (e.g., 90 MHz shift for 10 cm stretch). Furthermore, the effect of resonator coil pitch on the extension sensor gain (MHz cm−1) and linear span of the sensor is studied. The repeatability of the sensor gain is confirmed by performing hysteresis cycles. The sensors is coated with polydimethylsiloxane films to protect from electrical shorting in aqueous environments. The coated resonators are placed in a pipe to report flow rates. The sensor with 1 mm coating is found to have the largest gain (0.17 MHz⋅s mL−1) and linear span (10–100 mL s−1). Thus, flexible resonant sensors with kirigami‐inspired patterns can be tuned via geometric and coating considerations to wirelessly report a large range of extension lengths for potential uses in health monitoring, motion tracking, deformation detection, and soft robotics.more » « less
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