All forms of energy follow the law of conservation of energy, by which they can be neither created nor destroyed. Light-to-heat conversion as a traditional yet constantly evolving means of converting light into thermal energy has been of enduring appeal to researchers and the public. With the continuous development of advanced nanotechnologies, a variety of photothermal nanomaterials have been endowed with excellent light harvesting and photothermal conversion capabilities for exploring fascinating and prospective applications. Herein we review the latest progresses on photothermal nanomaterials, with a focus on their underlying mechanisms as powerful light-to-heat converters. We present an extensive catalogue of nanostructured photothermal materials, including metallic/semiconductor structures, carbon materials, organic polymers, and two-dimensional materials. The proper material selection and rational structural design for improving the photothermal performance are then discussed. We also provide a representative overview of the latest techniques for probing photothermally generated heat at the nanoscale. We finally review the recent significant developments of photothermal applications and give a brief outlook on the current challenges and future directions of photothermal nanomaterials.

https://pubs.acs.org/doi/pdf/10.1021/acs.chemrev.3c00159

Photothermal Nanomaterials: A Powerful Light-to-Heat Converter

Snap‐through bistability is often observed in nature (e.g., fast snapping to closure of Venus flytrap) and the life (e.g., bottle caps and hair clippers). Recently, harnessing bistability and multistability in different structures and soft materials has attracted growing interest for high‐performance soft actuators and soft robots. They have demonstrated broad and unique applications in high‐speed locomotion on land and under water, adaptive sensing and fast grasping, shape reconfiguration, electronics‐free controls with a single input, and logic computation. Here, an overview of integrating bistable and multistable structures with soft actuating materials for diverse soft actuators and soft/flexible robots is given. The mechanics‐guided structural design principles for five categories of basic bistable elements from 1D to 3D (i.e., constrained beams, curved plates, dome shells, compliant mechanisms of linkages with flexible hinges and deformable origami, and balloon structures) are first presented, alongside brief discussions of typical soft actuating materials (i.e., fluidic elastomers and stimuli‐responsive materials such as electro‐, photo‐, thermo‐, magnetic‐, and hydro‐responsive polymers). Following that, integrating these soft materials with each category of bistable elements for soft bistable and multistable actuators and their diverse robotic applications are discussed. To conclude, perspectives on the challenges and opportunities in this emerging field are considered.

Bistable and Multistable Actuators for Soft Robots: Structures, Materials, and Functionalities

Colloidal self-assembly refers to a solution-processed assembly of nanometer-/micrometer-sized, well-dispersed particles into secondary structures, whose collective properties are controlled by not only nanoparticle property but also the superstructure symmetry, orientation, phase, and dimension. This combination of characteristics makes colloidal superstructures highly susceptible to remote stimuli or local environmental changes, representing a prominent platform for developing stimuli-responsive materials and smart devices. Chemists are achieving even more delicate control over their active responses to various practical stimuli, setting the stage ready for fully exploiting the potential of this unique set of materials. This review addresses the assembly of colloids into stimuli-responsive or smart nanostructured materials. We first delineate the colloidal self-assembly driven by forces of different length scales. A set of concepts and equations are outlined for controlling the colloidal crystal growth, appreciating the importance of particle connectivity in creating responsive superstructures. We then present working mechanisms and practical strategies for engineering smart colloidal assemblies. The concepts underpinning separation and connectivity control are systematically introduced, allowing active tuning and precise prediction of the colloidal crystal properties in response to external stimuli. Various exciting applications of these unique materials are summarized with a specific focus on the structure-property correlation in smart materials and functional devices. We conclude this review with a summary of existing challenges in colloidal self-assembly of smart materials and provide a perspective on their further advances to the next generation.

Colloidal Self-Assembly Approaches to Smart Nanostructured Materials.

Bioinspired smart materials with synergistic allochroic luminescence and complex deformation are expected to play an important role in many areas of science and technology. However, it is still challenging to fabricate such soft actuators with high programmability that can be manipulated in situ with high spatial resolution. Herein, we have incorporated terminally functionalized aggregation-induced emission active tetraphenylethene derivative and photochromic spiropyran moieties into the networks of liquid crystal elastomers through covalent bonding to obtain the synergistic photochromic luminescence and programmable soft actuators. Bio-mimic functions and light-induced auxetic metamaterial-like devices were shown to be feasible based on the combination of assembly and origami-programming strategy. These bioinspired devices with synergistic photochromic luminescence and complex photodeformation abilities provide an elegant strategy to design multi-functional liquid crystal actuators.

Bioinspired Synergistic Photochromic Luminescence and Programmable Liquid Crystal Actuators

This review considers the most recent developments in supramolecular and supraparticle structures obtained from natural, renewable biopolymers as well as their disassembly and reassembly into engineered materials. We introduce the main interactions that control bottom-up synthesis and top-down design at different length scales, highlighting the promise of natural biopolymers and associated building blocks. The latter have become main actors in the recent surge of the scientific and patent literature related to the subject. Such developments make prominent use of multicomponent and hierarchical polymeric assemblies and structures that contain polysaccharides (cellulose, chitin, and others), polyphenols (lignins, tannins), and proteins (soy, whey, silk, and other proteins). We offer a comprehensive discussion about the interactions that exist in their native architectures (including multicomponent and composite forms), the chemical modification of polysaccharides and their deconstruction into high axial aspect nanofibers and nanorods. We reflect on the availability and suitability of the latter types of building blocks to enable superstructures and colloidal associations. As far as processing, we describe the most relevant transitions, from the solution to the gel state and the routes that can be used to arrive to consolidated materials with prescribed properties. We highlight the implementation of supramolecular and superstructures in different technological fields that exploit the synergies exhibited by renewable polymers and biocolloids integrated in structured materials.

Deconstruction and Reassembly of Renewable Polymers and Biocolloids into Next Generation Structured Materials.

Liquid crystal elastomers (LCEs) are of interest for applications such as soft robotics and shape-morphing devices. Among the different actuation mechanisms, light offers advantages such as spatial and local control of actuation via the photothermal effect. However, the unwanted aggregation of the light-absorbing nanoparticles in the LCE matrix will limit the photothermal response speed, actuation performance, and repeatability. Herein, a near-infrared-responsive LCE composite consisting of up to 0.20 wt% poly(ethylene glycol)-modified gold nanorods (AuNRs) without apparent aggregation is demonstrated. The high Young's modulus, 20.3 MPa, and excellent photothermal performance render repeated and fast actuation of the films (actuation within 5 s and recovery in 2 s) when exposed to 800 nm light at an average output power of ≈1.0 W cm-2 , while maintaining a large actuation strain (56%). Further, it is shown that the same sheet of AuNR/LCE film (100 µm thick) can be morphed into different shapes simply by varying the motifs of the photomasks.

Repeatable and Reprogrammable Shape Morphing from Photoresponsive Gold Nanorod/Liquid Crystal Elastomers.

Direct ink writing of liquid crystal elastomers (LCEs) offers a new opportunity to program geometries for a wide variety of shape transformation modes toward applications such as soft robotics. So far, most 3D‐printed LCEs are thermally actuated. Herein, a 3D‐printable photoresponsive gold nanorod (AuNR)/LCE composite ink is developed, allowing for photothermal actuation of the 3D‐printed structures with AuNR as low as 0.1 wt.%. It is shown that the printed filament has a superior photothermal response with 27% actuation strain upon irradiation to near‐infrared (NIR) light (808 nm) at 1.4 W cm−2 (corresponding to 160 °C) under optimal printing conditions. The 3D‐printed composite structures can be globally or locally actuated into different shapes by controlling the area exposed to the NIR laser. Taking advantage of the customized structures enabled by 3D printing and the ability to control locally exposed light, a light‐responsive soft robot is demonstrated that can climb on a ratchet surface with a maximum speed of 0.284 mm s−1 (on a flat surface) and 0.216 mm s−1 (on a 30° titled surface), respectively, corresponding to 0.428 and 0.324 body length per min, respectively, with a large body mass (0.23 g) and thickness (1 mm).

3D‐Printed Photoresponsive Liquid Crystal Elastomer Composites for Free‐Form Actuation

Liquid crystal elastomer (LCE) fibers exhibit large deformation and reversibility, making them an ideal candidate for soft actuators. It is still challenging to develop a scalable strategy and endow fiber actuators with photoelectric functions to achieve tailorable photo-electro-thermal responsiveness and rapid large actuation deformation. Herein, we fabricated a multiresponsive actuator that consists of LCE long fibers obtained by continuous dry spinning and further coated it with polydopamine (PDA)-modified MXene ink. The designed PDA@MXene-integrated LCE fiber is used for shape-deformable and multi-trigger actuators that can be photo- and electro-thermally actuated. The proposed LCE fiber actuator combines an excellent photothermal and long-term electrically conductive PDA@MXene and a shape-morphing LCE fiber, enabling their robust mechanical flexibility, multiple fast responses (∼0.4 s), and stable and large actuation deformation (∼60%). As a proof-of-concept, we present near-infrared light-driven artificial muscle that can lift 1000 times the weight and an intelligent circuit switch with stable controllability and fast responsiveness (∼0.1 s). Importantly, an adaptive smart window system that integrates light-driven energy harvesting/conversion functions is ingeniously constructed by the integration of a propellable curtain woven by the designed fiber and solar cells. This work can provide insights into the development of advanced intelligent materials toward soft robotics, sustainable energy savings and beyond.

Scalable functionalized liquid crystal elastomer fiber soft actuators with multi-stimulus responses and photoelectric conversion.

A ubiquitous structural feature in biological systems is texture in extracellular matrix that gains functions when hardened, for example, cell walls, insect scales, and diatom tests. Here, we develop patterned liquid crystal elastomer (LCE) particles by recapitulating the biophysical patterning mechanism that forms pollen grain surfaces. In pollen grains, a phase separation of extracellular material into a pattern of condensed and fluid-like phases induces undulations in the underlying elastic cell membrane to form patterns on the cell surface. In this work, LCE particles with variable surface patterns were created through a phase separation of liquid crystal oligomers (LCOs) droplet coupled to homeotropic anchoring at the droplet interface, analogously to the pollen grain wall formation. Specifically, nematically ordered polydisperse LCOs and isotropic organic solvent (dichloromethane) phase-separate at the surface of oil-in-water droplets, while, different LCO chain lengths segregate to different surface curvatures simultaneously. This phase separation, which creates a distortion in the director field, is in competition with homeotropic anchoring induced by sodium dodecyl sulfate (SDS). By tuning the polymer chemistry of the system, we are able to influence this separation process and tune the types of surface patterns in these pollen-like microparticles. Our study reveals that the energetically favorable biological mechanism can be leveraged to offer simple yet versatile approaches to synthesize microparticles for mechanosensing, tissue engineering, drug delivery, energy storage, and displays.

https://www.pnas.org/content/pnas/117/18/9699.full.pdf

Mimicry of a biophysical pathway leads to diverse pollen-like surface patterns

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Repeatable and Reprogrammable Shape Morphing from Photoresponsive Gold Nanorod/Liquid Crystal Elastomers.

3D‐Printed Photoresponsive Liquid Crystal Elastomer Composites for Free‐Form Actuation

Scalable functionalized liquid crystal elastomer fiber soft actuators with multi-stimulus responses and photoelectric conversion.

Mimicry of a biophysical pathway leads to diverse pollen-like surface patterns