Hydrogel-based MAMs are the most diverse and intensely studied, and have potential to be programmed with various responding behaviors and have broad applications in areas ranging from biomedical engineering to robotics. Hydrogel programmability, in some literature, refers to the fine-tuning of hydrogel deformation patterns. [4] Other works define programmability of hydrogels as molecular sequencing or arrangement within gel networks. [5] To provide a more consistent overview of programmable hydrogelbased MAMs, this review defines programmability as the ability to tune the input-output response function of the MAMs through either molecular design or patterning of the material across multiple length scales. There are MAMs that are responsive but the response function cannot be easily altered or tuned. For example, a conventional hydrogel can swell and deswell by controlling the humidity. But without spatially patterning the material or without doping certain copolymers into the gel, this type of conventional material is not inherently programmable. We will further discuss the approaches to integrate programmability into MAMs in Section 3.In this review, we first describe the chemical components of hydrogel-based MAMs and their fabrication, followed by specific approaches toward programmability. Then, a detailed classification of responsivity mechanisms is provided, along with discussion of the intimate relationships between material structure and their responsive behaviors. We then end by summarizing current applications of MAMs across multiple disciplines, and the future directions and applications of mechanically responsive hydrogels.
Components of HydrogelsMechanical responsivity has been observed in nearly all types of materials both hard and soft materials, spanning from metals to ceramics and polymers. Popular examples include shape-memory metal alloys, [6] piezoelectric ceramics, [7] and thermoresponsive polymers. [8] Herein, we will exlusively discuss programmable MAMs that are primarily composed of polymer hydrogels. This is because hydrogel materials are great candidates for flexible devices and bioengineering studies, and this has inspired multidisciplinary research and numerous potential applications. To be more consistent, inorganic nanoparticles, plastic, rubber, ceramics, polymer micelles/capsules, will not be discussed here since these types of materials are not hydrogels. Programmable mechanically active materials (MAMs) are defined as materials that can sense and transduce external stimuli into mechanical outputs or conversely that can detect mechanical stimuli and respond through an optical change or other change in the appearance of the material. Programmable MAMs are a subset of responsive materials and offer potential in next generation robotics and smart systems. This review specifically focuses on hydrogel-based MAMs because of their mechanical compliance, programmability, biocompatibility, and cost-efficiency. First, the composition of hydrogel MAMs along with the top-down and bottom-up a...