Light-induced shape morphing of thin films

Shape transformation of thin two-dimensional sheets into three-dimensional structures using light is of great interest for remotely controlled fabrication, surface modulation, and actuation. Over the last few decades, significant efforts have been made to develop material systems incorporating photochemical or photothermal elements to drive deformation in response to illumination. However, the full extent of the interplay between chemistry, optics, and mechanics in these materials is poorly understood. In this review, we introduce principles of shape morphing in these systems by considering the underlying physics of photoinduced stresses and how these have been used in recent literature. In addition, we provide a critical overview of the important design characteristics of both photochemical and photothermal system and offer our view on the open opportunities and challenges in this rapidly growing field

Liquid Crystal Elastomer Waveguide Actuators

While most photomechanical materials developed to date have relied on free‐space illumination to drive actuation, this strategy fails when direct line‐of‐site access is precluded. In this study, waveguided light is harnessed by liquid crystal elastomer (LCE) nanocomposites to drive actuation. Using photo‐chemical reduction of gold salts to plasmonic nanoparticles, prescription of photoresponsive regions within fibers of mono‐domain LCEs is demonstrated with control over both the location along the fiber axis, as well as in the azimuthal direction. Due to localized photothermal heating provided by plasmonic absorption of waveguided light and resulting inhomogeneous thermally induced deformation of the LCE, reversible bending along multiple axes is demonstrated

Complex Coacervation of Polymerized Ionic Liquids in Non-acqueous Solvents

Oppositely charged polymerized ionic liquids (PILs) were used to form complex coacervates in two different organic solvents, 2,2,2-trifluoroethanol (TFE) and hexafluoro-2-propanol (HFIP), and the corresponding phase diagrams were constructed using UV–vis, NMR, and turbidity experiments. While previous studies on complex coacervates have focused almost exclusively on aqueous environments, the use of PILs in the current work enabled studies in solvents with substantially lower dielectric constants (27.0 for TFE, 16.7 for HFIP). The critical salt concentration required to induce complete miscibility was roughly 2-fold larger in HFIP compared with TFE, and two different PIL complexes, solidlike precipitates and liquidlike coacervates, were found in both systems. This study provides insight into the effects of low-dielectric-constant solvents on complex coacervation, which has not been widely studied because of the limited solubility of conventional polyelectrolytes in these media

Controlled formation and disappearance of creases

Soft, elastic materials are capable of large and reversible deformation, readily leading to various modes of instability that are often undesirable, but sometimes useful. For example, when a soft elastic material is compressed, its initially flat surface will suddenly form creases. While creases are commonly observed, and have been exploited to control chemical patterning, enzymatic activity, and adhesion of surfaces, the conditions for the formation and disappearance of creases have so far been poorly controlled. Here we show that a soft elastic bilayer can snap between the flat and creased states repeatedly, with hysteresis. The strains at which the creases form and disappear are highly reproducible, and are tunable over a large range, through variations in the level of pre-compression applied to the substrate and the relative thickness of the film. The introduction of bistable flat and creased states and hysteretic switching is an important step to enable applications of this type of instability.Engineering and Applied Science

The role of substrate pre-stretch in post-wrinkling bifurcations

When a stiff film on a soft substrate is compressed, the surface of the film forms wrinkles, with tunable wavelengths and amplitudes that enable a variety of applications. As the compressive strain increases, the film undergoes post-wrinkling bifurcations, leading to period doubling and eventually to formation of localized folds or ridges. Here we study the post-wrinkling bifurcations in films on pre-stretched substrates. Through a combination of experiments and simulations, we demonstrate that pre-stretched substrates not only show substantial shifts in the critical strain for the onset of post-wrinkling bifurcations, but also exhibit qualitatively different post-wrinkled states. In particular, we report on the stabilization of wrinkles in films on pre-tensioned substrates and the emergence of ‘chaotic’ morphologies in films on pre-compressed substrates.Engineering and Applied Science

A nonlinear beam model of photomotile structures

Actuation remains a significant challenge in soft robotics. Actuation by light has important advantages: Objects can be actuated from a distance, distinct frequencies can be used to actuate and control distinct modes with minimal interference, and significant power can be transmitted over long distances through corrosion-free, lightweight fiber optic cables. Photochemical processes that directly convert photons to configurational changes are particularly attractive for actuation. Various works have reported light-induced actuation with liquid crystal elastomers combined with azobenzene photochromes. We present a simple modeling framework and a series of examples that study actuation by light. Of particular interest is the generation of cyclic or periodic motion under steady illumination. We show that this emerges as a result of a coupling between light absorption and deformation. As the structure absorbs light and deforms, the conditions of illumination change, and this, in turn, changes the nature of further deformation. This coupling can be exploited in either closed structures or with structural instabilities to generate cyclic motion

Reversible Actuation via Photoisomerization-Induced Melting of a Semicrystalline Poly(Azobenzene)

Photoisomerization of azobenzene in polymer matrices is a powerful method to convert photon energy into mechanical work. While most previous studies have focused on incorporating azobenzene within amorphous or liquid crystalline materials, the limited extents of molecular ordering and correspondingly modest enthalpy changes upon switching in such systems has limited the achievable energy densities. In this work, we introduce a semicrystalline main-chain poly(azobenzene), where photoisomerization is capable of reversibly triggering melting and recrystallization under essentially isothermal conditions. These materials can be drawn into aligned fibers, yielding optically driven two-way shape memory actuators capable of reversible bending

Controlling the configuration space topology of mechanisms

Linkages are mechanical devices constructed from rigid bars and freely rotating joints studied both for their utility in engineering and as mathematical idealizations in a number of physical systems. Recently, there has been a resurgence of interest in designing linkages to perform certain tasks from the physics community. We describe a method to design the topology of the configuration space of a linkage by first identifying the manifold of critical points, then perturbing around such critical configurations. We then demonstrate our procedure by designing a mechanism to gate the propagation of a soliton in a Kane-Lubensky chain of interconnected rotors

Electrohydrodynamically patterned colloidal crystals

A method for assembling patterned crystalline arrays of colloidal particles using ultraviolet illumination of an optically-sensitive semiconducting anode while using the anode to apply an electronic field to the colloidal particles. The ultraviolet illumination increases current density, and consequently, the flow of the colloidal particles. As a result, colloidal particles can be caused to migrate from non-illuminated areas of the anode to illuminated areas of the anode. Selective illumination of the anode can also be used to permanently affix colloidal crystals to illuminated areas of the anode while not affixing them to non-illuminated areas of the anode

Reconfiguring Gaussian Curvature of Hydrogel Sheets with Photoswitchable Host–Guest Interactions

Photoinduced shape morphing has implications in fields ranging from soft robotics to biomedical devices. Despite considerable effort in this area, it remains a challenge to design materials that can be both rapidly deployed and reconfigured into multiple different three-dimensional forms, particularly in aqueous environments. In this work, we present a simple method to program and rewrite spatial variations in swelling and, therefore, Gaussian curvature in thin sheets of hydrogels using photoswitchable supramolecular complexation of azobenzene pendent groups with dissolved α-cyclodextrin. We show that the extent of swelling can be programmed via the proportion of azobenzene isomers, with a 60% decrease in areal swelling from the all trans to the predominantly cis state near room temperature. The use of thin gel sheets provides fast response times in the range of a few tens of seconds, while the shape change is persistent in the absence of light thanks to the slow rate of thermal cis–trans isomerization. Finally, we demonstrate that a single gel sheet can be programmed with a first swelling pattern via spatially defined illumination with ultraviolet light, then erased with white light, and finally redeployed with a different swelling pattern