Molecular Rationale for the Design of Instantaneous, Strain-Tolerant Polymeric Adhesive in a Stretchable Underwater Human-Machine Interface.

Strain-tolerant reversible adhesion under harsh mechanical deformation is important for realizing long-lasting polymeric adhesives. Despite recent advances, cohesive failure within adhesives remains a critical problem that must be solved to achieve adhesion that is robust against humidity, heat, and mechanical stress. Here, we report a molecular rationale for designing an instantaneous polymeric adhesive with high strain tolerance (termed as iPASTE) even in a stretchable human-machine interface. The iPASTE consists of two biocompatible and eco-friendly polymers, linearly oligomerized green tea extracts, and poly(ethylene glycol) for densely assembled networks via dynamic and reversible hydrogen bonds. Other than the typical approach containing nanoclay or branched adhesive precursors, the linear configuration and conformation of such polymer chains within iPASTE lead to strong and moisture-resistant cohesion/adhesion. Based on the strain-tolerant adhesion of iPASTE, it was demonstrated that a subaqueous interactive human-machine interface integrated with a robot arm and a gold nanomembrane strain-sensitive electronic skin can precisely capture a slithery artificial fish by using finger gesture recognition.

Balanced Coexistence of Reversible and Irreversible Covalent Bonds in a Conductive Triple Polymeric Network Enables Stretchable Hydrogels with High Toughness and Adhesiveness.

The application of soft hydrogels to stretchable devices has attracted increasing attention in deformable bioelectronics owing to their unique characteristic, "modulus matching between materials and organs". Despite considerable progress, their low toughness, low conductivity, and absence of tissue adhesiveness remain substantial challenges associated with unstable skin-interfacing, where body movements undesirably disturb electrical signal acquisitions. Herein, we report a material design of a highly tough strain-dissipative and skin-adhesive conducting hydrogel fabricated through a facile one-step sol-gel transition and its application to an interactive human-machine interface. The hydrogel comprises a triple polymeric network where irreversible amide linkage of polyacrylamide with alginate and dynamic covalent bonds entailing conjugated polymer chains of poly(3,4-ethylenedioxythiophene)-co-(3-thienylboronic acid) are simultaneously capable of high stretchability (1300% strain), efficient strain dissipation (36,209 J/m2), low electrical resistance (590 Ω), and even robust skin adhesiveness (35.0 ± 5.6 kPa). Based on such decent characteristics, the hydrogel was utilized as a multifunctional layer for successfully performing either electrophysiological cardiac/muscular on-skin sensors or an interactive stretchable human-machine interface.

Stretchable colour-sensitive quantum dot nanocomposites for shape-tunable multiplexed phototransistor arrays.

High-performance photodetecting materials with intrinsic stretchability and colour sensitivity are key requirements for the development of shape-tunable phototransistor arrays. Another challenge is the proper compensation of optical aberrations and noises generated by mechanical deformation and fatigue accumulation in a shape-tunable phototransistor array. Here we report rational material design and device fabrication strategies for an intrinsically stretchable, multispectral and multiplexed 5 × 5 × 3 phototransistor array. Specifically, a unique spatial distribution of size-tuned quantum dots, blended in a semiconducting polymer within an elastomeric matrix, was formed owing to surface energy mismatch, leading to highly efficient charge transfer. Such intrinsically stretchable quantum-dot-based semiconducting nanocomposites enable the shape-tunable and colour-sensitive capabilities of the phototransistor array. We use a deep neural network algorithm for compensating optical aberrations and noises, which aids the precise detection of specific colour patterns (for example, red, green and blue patterns) both under its flat state and hemispherically curved state (radius of curvature of 18.4 mm).