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Abstract Most triblock copolymer-based physical hydrogels form three-dimensional networks through micellar packing, and formation of polymer loops represents a topological defect that diminishes hydrogel elasticity. This effect can be mitigated by maximizing the fraction of elastically effective bridges in the hydrogel network. Herein, we report hydrogels constructed by complexing oppositely charged multiblock copolymers designed with a sequence pattern that maximizes the entropic and enthalpic penalty of micellization. These copolymers self-assemble into branched and bridge-rich network units (netmers), instead of forming sparsely interlinked micelles. We find that the storage modulus of the netmer-based hydrogel is 11.5 times higher than that of the micelle-based hydrogel. Complementary coarse grained molecular dynamics simulations reveal that in the netmer-based hydrogels, the numbers of charge-complexed nodes and mechanically reinforcing bridges increase substantially relative to micelle-based hydrogels.

Abstract Copper (Cu) is widely used as an industrial electrode due to its high electrical conductivity, mechanical properties, and cost‐effectiveness. However, Cu is susceptible to corrosion, which degrades device performance over time. Although various methods (alloying, physical passivation, surface treatment, etc.) are introduced to address the corrosion issue, they can cause decreased conductivity or vertical insulation. Here, using the nitrogen‐doped amorphous carbon (a‐C:N) thin film is proposed as a substrate on which Cu is directly deposited. This simple method significantly inhibits corrosion of ultrathin Cu (

Abstract Deformable and miniaturized energy storage devices are essential for powering soft electronics. Herein, we fabricate deformable micro supercapacitors (MSCs) based on eutectic gallium-indium liquid metal (EGaIn) current collectors with integrated graphene. The well-define interdigitated electrode patterning with controlled gap is successfully realized by using the laser ablation because of a strong laser absorption of graphene and EGaIn. By judicious control of gap size between neighboring interdigitated electrodes and mass loading of graphene, we achieve a high areal capacitance (1336 µF cm−2) with reliable rate performance. In addition, owing to the intrinsic liquid characteristics of EGaIn current collector, the areal capacitance of fabricated MSC retains 90% of original value even after repetitive folding and 20% stretching up to 1000 cycles. Finally, we successfully integrate deformable MSC with a commercial light-emitting diode to demonstrate the feasibility of MSC as a deformable power source. The fabricated MSCs operate stably under various mechanical deformations, including stretching, folding, twisting, and wrinkling.

Abstract Display form factors such as size and shape have been conventionally determined in consideration of usability and portability. The recent trends requiring wearability and convergence of various smart devices demand innovations in display form factors to realize deformability and large screens. Expandable displays that are foldable, multi-foldable, slidable, or rollable have been commercialized or on the edge of product launches. Beyond such two-dimensional (2D) expansion of displays, efforts have been made to develop three dimensional (3D) free-form displays that can be stretched and crumpled for use in realistic tactile sensation, artificial skin for robots, and on-skin or implantable displays. This review article analyzes the current state of the 2D and 3D deformable displays and discusses the technological challenges to be achieved for industrial commercialization.

Abstract Piezoelectric self‐powered sensors are promising platforms for wearable portable devices. Poly(vinylidene fluoride) (PVDF) and its copolymer derivatives are extensively explored as a soft piezoelectric material owing to their high piezoelectric coefficient, chemical thermal stability, biocompatibility, lightweight, and excellent flexibility. It is proved that the dominance of the electroactive (EA) β‐phase crystals versus the non‐electroactive α‐phase crystals is one of the key parameters to obtaining high piezoelectric performance of PVDF. Conventional methods, such as mechanical stretching, electrical poling, and high‐temperature annealing, are investigated to enhance the fraction of the β‐phase. Recently, embedding nanoscale fillers in the PVDF matrix has been investigated to further increase the β‐phase fraction and achieved considerable advances. The introduction of nanofillers is also advantageous in terms of improving the electrical conductivity and dielectric properties of PVDF, which are not readily obtained through conventional methods. This review introduces the principles of EA phase transformation in the presence of nanofillers and summarizes recent advances achieved by introducing various fillers, such as perovskites, oxide semiconductors, and 2D chalcogenides. The potential sensor applications of the PVDF nanocomposites responding to temperature, light, acoustic, and mechanical stimuli are reviewed. This review ends with the outlook of this new approach.

Abstract Although ion gels are attractive sensing materials for deformable epidermal sensors or implantable devices, their sensing performances are highly affected by environmental humidity change, so that their sensing reliability cannot be secured. This study proposes a new concept of maintaining the high‐precision temperature sensing performance of highly deformable ion gel sensors. In this approach, a hydrophobic ion gel sensing layer is kept water‐saturated by attaching a hydrogel layer, rather than attempting to completely block water penetration. This study performs experimental and theoretical investigation on water concentration in the ion gel, using the analysis of mass transportation at the interface of the ion gel and the hydrogel. By using the charge relaxation time of the ionic molecules, the temperature sensor is not affected by environmental humidity in the extreme range of humidity (30%–100%). This study demonstrates a highly deformable on‐skin temperature sensor which shows the same performance either in water or dry state and while exercising with large strains (ε = 50%).

Abstract Stretchable electronics has emerged over the past decade and is now expected to bring form factor‐free innovation in the next‐generation electronic devices. Stretchable devices have evolved with the synthesis of new soft materials and new device architectures that require significant deformability while maintaining the high device performance of the conventional rigid devices. As the mismatch in the mechanical stiffness between materials, layers, and device units is the major challenge for stretchable electronics, interface control in varying scales determines the device characteristics and the level of stretchability. This article reviews the recent advances in interface control for stretchable electronic devices. It summarizes the design principles and covers the representative approaches for solving the technological issues related to interfaces at different scales: i) nano‐ and microscale interfaces between materials, ii) mesoscale interfaces between layers or microstructures, and iii) macroscale interfaces between unit devices, substrates, or electrical connections. The last section discusses the current issues and future challenges of the interfaces for stretchable devices.