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Soft-bodied aquatic organisms exhibit extraordinary navigation and mobility in liquid environments which inspiring the development of biomimetic actuators with complex movements. Stimulus-responsive soft materials including hydrogels and shape-memory polymers are replacing traditional rigid parts that leading to dynamic and responsive soft actuators. In this study, we took inspiration from water strider to develop a biomimetic actuator for targeted stimulation and pH sensing in the gastrointestinal tract. We designed a soft and water-based Janus adhesive hydrogel patch that attaches to specific parts of the intestine and responds to pH changes through external stimulation. The hydrogel patch that forms the belly of the water strider driver incorporates an inverse opal microstructure that enables pH responsive behavior. The hydrogel patch on the water strider's leg uses a sandwich structure of Cu particles to convert light into heat and bend under infrared light to mimic the water strider's leg simulating the efficient and steady movement of the water strider's leg which transporting the biological fluid in one direction. This miniature bionic actuator demonstrates controlled adhesion and unidirectional biofluid delivery capabilities, proving its potential for targeted stimulus response and pH sensing in the gastrointestinal tract, thus opening up new possibilities for medical applications in the growing field of soft actuators.

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Osteoporotic bone defects are serious medical problems due to their sparse bone structure, difficulty in restoration and reconstruction, and high recurrence rates, which also result in heavy economic and social burdens. Herein, we developed a hierarchical hydrogel composed of alendronate sodium (AS)/Mg2+-loaded inverse opal methylpropenylated gelatin (GelMA) hydrogel microspheres (IOHM-AS-Mgs) within methylpropenylated poly(hyaluronic acid) (HAMA) for osteoporotic bone defect treatment. The IOHM-AS-Mgs displayed good cytocompatibility and cell adhesion and strongly stimulated osteogenesis at the transcriptomic and protein levels. When this treatment was applied to the osteoporotic bone defect area, HAMA was used to fix the microspheres. The results of the microcomputed tomography (micro-CT) and histological analyses indicated that the hierarchical hydrogel had the best therapeutic effect. Therefore, this hydrogel is a new candidate for osteoporotic bone defect treatment.

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Electrophoretic displays (EPDs) based on photonic crystals show great potential due to their reduced eye fatigue and low power consumption. However, the current image quality and service life of this system still face great challenges. In this work, we fabricated a new kind of electrically responsive photonic crystal (ERPC) device based on PSMA@SiO2 liquid colloidal crystals (LCCs) for EPDs. By introduction of the PSMA core with lower density and higher refractive index, the suspension stability and color saturation of PSMA@SiO2 LCCs were greatly enhanced compared with those of bare SiO2 LCCs. The PSMA@SiO2 LCCs showed brilliant colors, wide color tuning range (∼200 nm), and good reversibility under low voltages (<4 V). Interestingly, the transparency of PSMA@SiO2 LCCs could also be obviously regulated by an electric field, which was different from the traditional ways that change the thickness of PCs or contrast of refractive index (Δn) between the nanospheres and matrix. This transparency modulation offered a novel idea for the transmittance control of smart windows. As a proof of concept, we fabricated a new type of patterned ERPC device to demonstrate their potential in electrophoretic displays and smart windows with controllable transmittance under an electric field.

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Soft-bodied aquatic organisms have exhibited remarkable capabilities in navigating and moving within liquid environments serving as a profound inspiration for the development of bionic robots with intricate movements. Traditional rigid components are being replaced by stimulus-responsive soft materials such as hydrogels and shape memory polymers, leading to the creation of dynamically responsive soft robots. In this study, the development of a bionic robot inspired by the shape of an octopus and the adsorptive properties of its tentacles, specifically tailored for targeted stimulation and pH sensing in the cervix, are presented. This approach involves the design of a soft, water-based Janus adhesive hydrogel patch that adheres to specific parts of the cervix and responds to pH changes through external stimuli. The hydrogel patch incorporates inverse opal microstructures mimicking the legs of an octopus, to facilitate efficient and stable locomotion, unidirectional transport of biofluids, and pH-responsive behavior. This miniature bionic robot showcases controlled adhesion and precise unidirectional fluid transport highlighting its potential for targeted stimulus response and pH sensing in the uterine cervical tract. This breakthrough opens new avenues for medical applications within the expanding field of soft-bodied robotics.

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Attractive depletion interactions are utilized to organize colloidal particles into crystalline arrays with high crystallinity through spontaneous phase separation. However, uncontrolled nucleation frequently leads to the formation of crystalline grains with varied crystal orientations, which hampers the optical performance of photonic crystals. Here, colloidal crystals have been engineered with uniform orientation and high surface coverage by applying centrifugal force during the depletion-induced assembly of polystyrene particles. The centrifugal force encourages the particles to move toward the bottom surface, which fosters heterogeneous nucleation and supports rapid crystal growth, yielding densely-packed and uniformly-arranged crystal grains with high reflectivity. This study has observed that the nucleation and crystal growth behavior is significantly influenced by the salt concentration. Based on the pair potentials, the transition boundary has been quantitatively analyzed between fluid and crystal phases and identified the threshold for homogeneous nucleation. Utilizing the high-reflectivity colloidal crystals, band-edge lasing is achieved by dissolving the water-soluble dye into the aqueous suspensions. Upon optical excitation, a lasing emission characterized is observed by a narrow spectral width at the short-wavelength band edge. Notably, the laser wavelength can be adjusted by altering the salt concentration or particle diameter, offering a versatile approach to tuning the optical properties.

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Nanoparticle assembly is a material synthesis strategy that enables precise control of nanoscale structural features. Concepts from traditional crystal growth research have been tremendously useful in predicting and programming the unit cell symmetries of these assemblies, as their thermodynamically favored structures are often identical to atomic crystal analogues. However, these analogies have not yielded similar levels of influence in programming crystallite shapes, which are a consequence of both the thermodynamics and kinetics of crystal growth. Here, we demonstrate kinetic control of the colloidal crystal shape using nanoparticle building blocks that rapidly assemble over a broad range of concentrations, thereby producing well-defined crystal habits with symmetrically oriented dendritic protrusions and providing insight into the crystals' morphological evolution. Counterintuitively, these nonequilibrium crystal shapes actually become more common for colloidal crystals synthesized closer to equilibrium growth conditions. This deviation from typical crystal growth processes observed in atomic or molecular crystals is shown to be a function of the drastically different time scales of atomic and colloidal mass transport. Moreover, the particles are spherical with isotropic ligand grafts, and these kinetic crystal habits are achieved without the need for specifically shaped particle building blocks or external templating or shape-directing agents. Thus, this work provides generalizable design principles to expand the morphological diversity of nanoparticle superlattice crystal habits beyond the anhedral or equilibrium polyhedral shapes synthesized to date. Finally, we use this insight to synthesize crystallite shapes that have never before been observed, demonstrating the ability to both predict and program kinetically controlled superlattice morphologies.

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Printing structurally colored patterns is of great importance for providing customized graphics for various purposes. Although a direct writing technique has been developed, the use of colloidal dispersions as photonic inks requires delicate printing conditions and restricts the mechanical and optical properties of printed patterns. In this work, we produce elastic photonic microbeads through scalable bulk emulsification and formulate photonic inks containing microbeads for direct writing. To produce the microbeads, a photocurable colloidal dispersion is emulsified into a highly concentrated sucrose solution via vortexing, which results in spherical emulsion droplets with a relatively narrow size distribution. The microbeads are produced by photopolymerization and are then suspended in urethane acrylate resin at volume fractions of 0.35-0.45. The photonic inks retain high color saturation of the microbeads and offer enhanced printability and dimensional control on various target substrates including fabrics, papers, and even skins. Importantly, the printed graphics show high mechanical stability as the elastic microbeads are embedded in the polyurethane matrix. Moreover, the colors show a wide viewing angle and low-angle dependency due to the optical isotropy of individual microbeads and light refraction at the air-matrix interface. We postulate that this versatile direct writing technique is potentially useful for structural color coating and printing on the surfaces of arbitrary 3D objects.

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In the quest to develop advanced monitoring systems for intestinal peristaltic stress, this study introduces a groundbreaking approach inspired by nature's sensory networks. By the integration of novel materials and innovative manufacturing techniques, a multifunctional Janus hydrogel patch has been engineered. This unique patch not only demonstrates superior stress-sensing capabilities in the intricate intestinal environment but also enables adhesion to wet tissue surfaces. This achievement opens new avenues for real-time physiological monitoring and potential therapeutic interventions in the realm of gastrointestinal health.

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Transformable mechanical structures can switch between distinct mechanical states. Whether this kind of structure can be self-assembled from simple building blocks at microscale is a question to be answered. In this work, we propose a self-assembly strategy for these structures based on a nematic monolayer of segmented colloidal rods with lateral cutting. By using Monte Carlo simulation, we find that rods with different cutting degrees can self-assemble into different crystals characterized by bond coordination z that varies from 3 to 6. Among these, we identify a transformable superisostatic structure with pgg symmetry and redundant bonds (z = 5). We show that this structure can support either soft bulk modes or soft edge modes depending on its Poisson's ratio, which can be tuned from positive to negative through a uniform soft deformation. We also prove that the bulk soft modes are associated with states of self-stress along the direction of zero strain during uniform soft deformation. The self-assembled transformable structures may act as mechanical metamaterials with potential applications in micromechanical engineering.

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Dendrites are ubiquitous crystals produced in supersaturated solutions and supercooled melts, but considerably less is known about their formation and growth kinetics. Here, the key factors are explored that dictate dendrite formation and growth, utilizing experimental colloidal models in which the particles act as molecules with Mie potential. Depletion attraction is employed to colloids and manipulate their strength to control supersaturation. Dendrites are predominantly produced under conditions of low supersaturation, where the separation between crystals is large due to slow nucleation. The dendrites do not emerge directly from nuclei. Instead, isotropic grains, initially produced from nuclei, morph into polygons. Arms then sprout from the vertices of these polygons, eventually giving rise to dendrites. Triggering this polygon-to-dendrite transformation requires a high diffusional flux. This necessitates a prolonged diffusion time to maintain a steep concentration gradient in the surrounding environment even after the transformation from circular grains to polygons.

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Tuning the lattice spacing or stop bands holds great significance in the design and application of materials with colloidal crystals. Typically, particle surface modifications or the application of external physical fields are needed. In this study, we demonstrated the ability to expand or compress the lattice of colloidal crystals simply by utilizing a salt solution, without the need for any special treatments to the colloidal particles. We found that by only considering the diffusiophoresis effect we cannot explain the reversion of lattice expansion to lattice compression with the increase in the salt concentration and that the diffusioosmotic flow originating from the container wall must be taken into account. Further analysis revealed that variations in the salt concentration altered the relative amplitudes between diffusiophoresis and diffusioosmosis through changing the zeta potentials of the particles and the wall, and the competition between the particle diffusiophoresis and wall diffusioosmosis lay at the center of the underlying mechanism.

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While stimuli-responsive structural colors are commonly found in nature, mimicking these in artificial materials is challenging. Dynamically switchable and tunable coloration, however, is in high demand in widespread fields of applications, including advanced display and monitoring technologies, smart sensing, and anticounterfeiting. This work reports a scalable protocol for the synthesis of tailor-made core-shell particles and subsequent processing to opal films with iridescent, pH-responsive, and mechanochromic structural color. Novel monodisperse core-shell architectures based on hard polystyrene core particles are synthesized via stepwise emulsion polymerization in a starved-feed mode. The incorporation of 4-vinylpyridine and methacrylic acid as functional comonomers in the soft particle shell facilitates pH-responsive swelling and deswelling. Mechanically stable and well-ordered colloidal crystal films are obtained by the self-assembly of the particles during processing with the powerful melt-shear organization technique. Thereby obtained opal films show Bragg-scattering at the colloidal crystalline structure and exhibit brilliant green-turquoise to blue-violet reflection colors, dependent on the angle of view and illumination. Upon changes in the pH value or mechanical deformation, the reflected wavelength shifts by more than 100 nm, leading to intriguing changes in the visible structural color. Excellent reversibility is achieved by the subsequent application of a convenient UV cross-linking strategy, corroborating the high application potential of these advanced functional materials.

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Colloidal crystals display photonic stopbands that generate reflective structural colors. While micropatterning offers significant value for various applications, the resolution is somewhat limited for conventional top-down approaches. In this work, a simple, single-step bottom-up approach is introduced to produce photonic micropatterns through depletion-mediated regioselective growth of colloidal crystals. Lithographically-featured micropatterns with planar surfaces and nano-needle arrays as substrates are employed. Heterogeneous nucleation is drastically suppressed on nano-needle arrays due to minimal particle-to-needles overlap of excluded volumes, while it is promoted on planar surfaces with large particle-to-plane volume overlap, enabling regioselective growth of colloidal crystals. This strategy allows high-resolution micropatterning of colloidal photonic crystals, with a minimum feature size as small as 10 µm. Stopband positions, or structural colors, are controllable through concentration and depletant and salt, as well as particle size. Notably, secondary colors can be created through structural color mixing by simultaneously crystallizing two different particle sizes into their own crystal grains, resulting in two distinct reflectance peaks at controlled wavelengths. The simple and highly reproducible method for regioselective colloidal crystallization provides a general route for designing elaborate photonic micropatterns suitable for various applications.

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In vivo surgical interventions require effective management of biofluids, including controlling bleeding and removing excess biofluids such as bile, wound exudate, and blood. To address these issues, recent advances have emerged, such as self-sealing needles, drug-eluting stents, and shear-thinning hydrogels. However, complications associated with intestinal mucosal injury and secondary damage still persist. Therefore, a multifunctional stent is urgently required that can effectively remove excessive biofluid. Surface wettability of biliary stents is crucial in biofluid management, and conventional coatings can cause adhesion to wound tissue. To overcome this issue, we developed an interpenetrating Janus wettability stent coating, enabling unidirectional draining of excessive biofluid from its hydrophobic side to hydrophilic side, thereby preventing biofluid from wetting the wound. Furthermore, we demonstrate a directional biofluid movement using a self-pumping dressing in an infected tissue model, providing a new approach for in situ biofluid collection and disease diagnosis by detecting metal ion changes. Overall, our integrated system presents an opportunity to design wound dressings with effective biofluid management and metal ion detection capabilities.

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Existing strategies designed to produce ordered arrangements of colloidal particles on solid supports are of great interest for their wide range of applications, from colloidal lithography, plasmonic and biomimetic surfaces to tags for anti-counterfeiting, but they all share various degrees of complexity hampering their facile implementation. Here, a drastically simplified methodology is presented to achieve ordered particle deposition, consisting in adding micromolar amounts of cationic surfactant to a colloidal suspension drop and let it evaporate in an upside-down configuration. Confinement at the air/water interface enables particle assembly into monolayers, which are then transferred on the substrate producing highly ordered structures displaying vivid, orientation-dependent structural colors. The method is compatible with many particle types and substrates, while controlling system parameters allows tuning the deposit size and morphology, from monocrystals to polycrystalline disks and "irises", from single-component to crystal alloys with Moiré patterns, demonstrating its practicality for a variety of processes.

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Colloids self-organize into icosahedral clusters composed of a Mackay core and an anti-Mackay shell under spherical confinement to minimize the free energy. This study explores the variation of surface arrangements of colloids in icosahedral clusters, focusing on the determining factors behind the surface arrangement. To efficiently assemble particles in emulsion droplets, droplet-to-droplet osmotic extraction from particle-laden droplets to salt-containing droplets is used, where the droplets are microfluidically prepared to guarantee a high size uniformity. The icosahedral clusters are optimally produced during a 24-h consolidation period at a 0.04 m salt concentration. The findings reveal an increase in the number of particle layers from 10 to 15 in the icosahedral clusters as the average number of particles increases from 3300 to 11 000. Intriguingly, the number of layers in the anti-Mackay shells, or surface termination, appears to more strongly depend on the sphericity of the clusters than on the deviation in the particle count from an ideal icosahedral cluster. This result suggests that the sphericity of the outermost layer, formed by the late-stage rearrangement of particles to form an anti-Mackay shell near the droplet interface, may play a pivotal role in determining the surface morphology to accommodate a spherical interface.

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Interferometry-based, reflectometric, label-free biosensors have made significant progress in the analysis of molecular interactions after years of development. The design of interference substrates is a key research topic for these biosensors, and many studies have focused on porous films prepared by top-down methods such as porous silicon and anodic aluminum oxide. Lately, more research has been conducted on ordered porous layer interferometry (OPLI), which uses ordered porous colloidal crystal films as interference substrates. These films are made using self-assembly techniques, which is the bottom-up approach. They also offer several advantages for biosensing applications, such as budget cost, adjustable porosity, and high structural consistency. This review will briefly explain the fundamental components of self-assembled materials and thoroughly discuss various self-assembly techniques in depth. We will also summarize the latest studies that used the OPLI technique for label-free biosensing applications and divide them into several aspects for further discussion. Then, we will comprehensively evaluate the strengths and weaknesses of self-assembly techniques and discuss possible future research directions. Finally, we will outlook the upcoming challenges and opportunities for label-free biosensing using the OPLI technique.

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Colloidal crystals are designed as photonic microparticles for various applications. However, conventional microparticles generally have only one stopband from a single lattice constant, which restricts the range of colors and optical codes available. Here, photonic microcapsules are created that contain two or three distinct crystalline grains, resulting in dual or triple stopbands that offer a wider range of colors through structural color mixing. To produce distinct colloidal crystallites from binary or ternary colloidal mixtures, the interparticle interaction is manipulated using depletion forces in double-emulsion droplets. Aqueous dispersions of binary or ternary colloidal mixtures in the innermost droplet are gently concentrated in the presence of a depletant and salt by imposing hypertonic conditions. Different-sized particles crystallize into their own crystals rather than forming random glassy alloys to minimize free energy. The average size of the crystalline grains can be adjusted with osmotic pressure, and the relative ratio of distinct grains can be controlled with the mixing ratio of particles. The resulting microcapsules with small grains and high surface coverage are almost optically isotropic and exhibit highly-saturated mixed structural colors and multiple reflectance peaks. The mixed color and reflectance spectrum are controllable with the selection of particle sizes and mixing ratios.

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Self-assembled colloidal crystals display structural colors due to light diffracted from their microscale, ordered structure. This color arises due to Bragg reflection (BR) or grating diffraction (GD); the latter mechanism is much less explored than the former. Here the design space for generating GD structural color is identified and its relative advantages are demonstrated. Electrophoretic deposition is used to self-assemble crystals with fine crystal grains from colloids of diameter 1.0 µm. The structural color in transmission is tunable across the full visible spectrum. The optimum optical response-represented by both color intensity and saturation-is observed at low layer number (≤5 layers). The spectral response is well predicted by Mie scattering of the crystals. Taken together, the experimental and theoretical results demonstrate that vivid grating colors with high color saturation can be produced from thin layers of micron-sized colloids. These colloidal crystals extend the potential of artificial structural color materials.

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Colloidal photonic crystals, which are three-dimensional periodic structures of monodisperse submicron-sized particles, are expected to be suitable for novel photonic applications and color materials. In particular, nonclose-packed colloidal photonic crystals immobilized in elastomers exhibit significant potential for use in tunable photonic applications and strain sensors that detect strain based on color change. This paper reports a practical method for preparing elastomer-immobilized nonclose-packed colloidal photonic crystal films with various uniform Bragg reflection colors using one kind of gel-immobilized nonclose-packed colloidal photonic crystal film. The degree of swelling was controlled by the mixing ratio of the precursor solutions, which used a mixture of solutions with high and low affinities for the gel film as the swelling solvent. This facilitated color tuning over a wide range, enabling the facile preparation of elastomer-immobilized nonclose-packed colloidal photonic crystal films with various uniform colors via subsequent photopolymerization. The present preparation method can contribute to the development of practical applications of elastomer-immobilized tunable colloidal photonic crystals and sensors.