Humidity-Controlled Tunable Emission in a Dye-Incorporated Metal-Hydrogel-Metal Cavity.

Actively controllable photoluminescence is potent for a wide variety of applications from biosensing and imaging to optoelectronic components. Traditionally, methods to achieve active emission control are limited due to complex fabrication processes or irreversible tuning. Here, we demonstrate active emission tuning, achieved by changing the ambient humidity in a fluorescent dye-containing hydrogel integrated into a metal-insulator-metal (MIM) system. Altering the overlapping region of the MIM cavity resonance and the absorption and emission spectra of the dye used is the underlying principle to achieving tunability of the emission. We first verify this by passive tuning of cavity resonance and further experimentally demonstrate active tuning in both air and aqueous environments. The proposed approach is reversible, easy to integrate, and spectrally scalable, thus providing opportunities for developing tunable photonic devices.

Humidity- and Temperature-Tunable Metal-Hydrogel-Metal Reflective Filters.

A tunable reflectance filter based on a metal-hydrogel-metal structure responsive to humidity and temperature is reported. The filter employs a poly(N-isopropylacrylamide)-acrylamidobenzophenone (PNIPAm-BP) hydrogel as an insulator layer in the metal-insulator-metal (MIM) assembly. The optical resonance of the structure is tunable by water immersion across the visible and near-infrared range. Swelling/deswelling and the volume phase transition of the hydrogel allow continuous reversible humidity- and/or temperature-induced tuning of the optical resonance. This work paves the way toward low-cost large-area fabrication of actively tunable reversible photonic devices.

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.

Tunable Photomechanics in Diarylethene-Driven Liquid Crystal Network Actuators.

The response of soft actuators made of stimuli-responsive materials can be phenomenologically described by a stimulus-deformation curve, depicting the controllability and sensitivity of the actuator system. Manipulating such stimulus-deformation curve allows fabricating soft microrobots with reconfigurable actuation behavior, which is not easily achievable using conventional materials. Here, we report a light-driven actuator based on a liquid crystal polymer network containing diarylethene (DAE) photoswitches as cross-links, in which the stimulus-deformation curve under visible-light illumination is tuned with UV light. The tuning is brought about by the reversible electrocyclization of the DAE units. Because of the excellent thermal stability of the visible-absorbing closed-form DAEs, the absorbance of the actuator can be optically fixed to a desired value, which in turn dictates the efficiency of photothermally induced deformation. We employ the controllability in devising a logical AND gate with macroscopic output, i.e., an actuator that bends negligibly under UV or visible light irradiation, but with profound shape change when addressed to both simultaneously. The results provide design tools for reconfigurable microrobotics and polymer-based logic gating.

Design principles for non-reciprocal photomechanical actuation.

Non-reciprocal motions are a sequence of movements exhibiting time-reversal asymmetry. Such movements are common among various natural species, being adopted as a typical strategy for achieving efficient locomotion. Generally, the realization of non-reciprocal motions in man-made robotic devices requires synchronous control of at least two individual actuators, hence posing challenges to soft micro-robotics where the miniaturization limits integration of different mechanical components and the possibility of using onboard batteries. Here, we introduce general concepts for achieving non-reciprocal movements in wirelessly controlled soft actuators made of photomechanically responsive liquid crystal networks. The monolithic actuators are composed of two segments that can be actuated photochemically and photothermally, and the non-reciprocal motion is obtained by a control sequence that temporally modulates light sources of different wavelengths. Through proper selection of photoactive compounds, the number of modulated light sources can be decreased, from three to two, and eventually to one. Finally, we demonstrate non-reciprocal self-oscillation by self-shadowing effect in a flexible strip under a constant light field with no temporal modulation. This study provides general guidelines to light-controlled non-reciprocal actuation, offering new strategies for the control of wireless soft micro-robotics.

Light-fuelled freestyle self-oscillators.

Self-oscillation is a phenomenon where an object sustains periodic motion upon non-periodic stimulus. It occurs commonly in nature, a few examples being heartbeat, sea waves and fluttering of leaves. Stimuli-responsive materials allow creating synthetic self-oscillators fuelled by different forms of energy, e.g. heat, light and chemicals, showing great potential for applications in power generation, autonomous mass transport, and self-propelled micro-robotics. However, most of the self-oscillators are based on bending deformation, thereby limiting their possibilities of being implemented in practical applications. Here, we report light-fuelled self-oscillators based on liquid crystal network actuators that can exhibit three basic oscillation modes: bending, twisting and contraction-expansion. We show that a time delay in material response dictates the self-oscillation dynamics, and realize a freestyle self-oscillator that combines numerous oscillation modes simultaneously by adjusting the excitation beam position. The results provide new insights into understanding of self-oscillation phenomenon and offer new designs for future self-propelling micro-robots.

Reconfigurable photoactuator through synergistic use of photochemical and photothermal effects.

A reconfigurable actuator is a stimuli-responsive structure that can be programmed to adapt different shapes under identical stimulus. Reconfigurable actuators that function without control circuitry and are fueled remotely are in great demand to devise adaptive soft robotic devices. Yet, obtaining fast and reliable reconfiguration remains a grand challenge. Here we report a facile fabrication pathway towards reconfigurability, through synergistic use of photochemical and photothermal responses in light-active liquid crystal polymer networks. We utilize azobenzene photoisomerization to locally control the cis-isomer content and to program the actuator response, while subsequent photothermal stimulus actuates the structure, leading to shape morphing. We demonstrate six different shapes reconfigured from one single actuator under identical illumination conditions, and a light-fueled smart gripper that can be commanded to either grip and release or grip and hold an object after ceasing the illumination. We anticipate this work to enable all-optical control over actuator performance, paving way towards reprogrammable soft micro-robotics.