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Graphene-based actuators featuring fast and reversible deformation under various external stimuli are promising for soft robotics. However, these bimorph actuators are incapable of complex and programmable 3D deformation, which limits their practical application. Here, inspired from the collective coupling and coordination of living cells, we fabricated a moisture-responsive graphene actuator swarm that has programmable shape-changing capability by programming the SU-8 patterns underneath. To get better control over the deformation, we fabricated SU-8 micropattern arrays with specific geometries and orientations on a continuous graphene oxide film, forming a swarm of bimorph actuators. In this way, predictable and complex deformations, including bending, twisting, coiling, asymmetric bending, 3D folding, and combinations of these, have been achieved due to the collective coupling and coordination of the actuator swarm. This work proposes a new way to program the deformation of bilayer actuators, expanding the capabilities of existing bimorph actuators for applications in various smart devices. [ABSTRACT FROM AUTHOR]

• A complementary strategy can work as a universal design principle for dual-responsive actuators. • Combining moisture-active/alkane-inert GO with alkane-active/moisture-inert PDMS enables dual-responsive actuation. • GO and PDMS bimorph features fast and reversible response to both moisture and alkane. Smart actuators that enable deforming in a predictable manner under external stimuli have revealed great potential for both traditional and emerging industries. Generally, an asymmetric bilayer structure with one layer active and the other inert to a certain stimulus is essential to realize bending behavior. However, towards the development of dual- or multi-responsive actuators, it still lacks universal and effective strategies for rational design and fabrication of such devices through the simplest way. In this paper, we report a complementary strategy to produce dual-responsive bilayer actuators by combining the moisture-active/alkane-inert graphene oxide (GO) layer with the alkane-active/moisture-inert polydimethylsiloxane (PDMS) layer. The GO@PDMS bimorph actuator can switch its active and inert layers in response to moisture and alkane, respectively, realizing dual-responsive deformation under different actuations. Typical dual-responsive actuators, including a selective air valve and a grip and hook smart claw, are successfully fabricated, demonstrating the capability of effective gases and objects transmission. The complementary bimorph actuator may hold great promise for developing intelligent devices and portable delivery systems. [ABSTRACT FROM AUTHOR]

Abstract: Actuators that can convert environmental stimuli into mechanical work are widely used in intelligent systems, robots, and micromechanics. To produce robust and sensitive actuators of different scales, efforts are devoted to developing effective actuating schemes and functional materials for actuator design. Carbon‐based nanomaterials have emerged as preferred candidates for different actuating systems because of their low cost, ease of processing, mechanical strength, and excellent physical/chemical properties. Especially, due to their excellent photothermal activity, which includes both optical absorption and thermal conductivities, carbon‐based materials have shown great potential for use in photothermal actuators. Herein, the recent advances in photothermal actuators based on various carbon allotropes, including graphite, carbon nanotubes, amorphous carbon, graphene and its derivatives, are reviewed. Different photothermal actuating schemes, including photothermal effect–induced expansion, desorption, phase change, surface tension gradient creation, and actuation under magnetic levitation, are summarized, and the light‐to‐heat and heat‐to‐work conversion mechanisms are discussed. Carbon‐based photothermal actuators that feature high light‐to‐work conversion efficiency, mechanical robustness, and noncontact manipulation hold great promise for future autonomous systems. [ABSTRACT FROM AUTHOR]

The combination of surface-enhanced Raman spectroscopy (SERS) technology with microfluidics makes it possible to diagnose genetic disease through label-free on-chip DNA detection. However, open problems including the integration of SERS substrate with microfluidic devices, controllable trapping and releasing of target molecules are still challenging. Here we demonstrate a facile laser scribing method to fabricate silver nanoparticles (AgNPs) and graphene oxide (GO) based biochips as a reusable SERS sensor for DNA detection. Programmable laser scribing of the AgNPs@GO composite film enables direct patterning of sensitive SERS channels that consist of graphene supported AgNPs by exfoliating the composites into hierarchical porous structures. Integrating the SERS-active patterns with a microfluidic chip forms a biochip for allowing SERS detection of DNA. The noncovalent interactions between DNA and graphene mediated controllable trapping and releasing of DNA sequences, enabling efficient on-chip SERS detection and the regeneration of the biochip. The simple, green and cost-effective fabrication of the SERS-active biochips reveals great potential for biomolecular sensing and genetic engineering applications. [ABSTRACT FROM AUTHOR]

This paper demonstrates femtosecond laser direct writing mediated flexible integration of plasmonic Ag/Pd alloy nanostructures that can be potentially used as a robust surface‐enhanced Raman spectroscopy substrate inside the microfluidic chip. Silver–palladium alloy with controllable composition ratio can be patterned into plasmonic nanostructures due to two‐photon absorption induced coreduction of silver/palladium double metal ions. Since the alloy structures can effectively protect the silver from oxidation, thus they can facilitate the stable on‐chip detection devices with long lifetime. The as‐fabricated silver–palladium alloy substrate with 18% content of palladium maintains a relatively high enhancement factor of about 2.62 × 108 while at the same time demonstrating the best stability against aerobic oxidation, as it is stable for up to 20 d under ambient aerobic conditions, exhibiting a significant improvement compared to those unprotected silver substrates which have a limited lifetime of only 3 or 4 d. [ABSTRACT FROM AUTHOR]

In the development of microfluidic chips, conventional 2D processing technologies contribute to the manufacturing of basic microchannel networks. Nevertheless, in the pursuit of versatile microfluidic chips, flexible integration of multifunctional components within a tiny chip is still challenging because a chip containing micro-channels is a non-flat substrate. Recently, on-chip laser processing (OCLP) technology has emerged as an appealing alternative to achieve chip functionalization through in situ fabrication of 3D microstructures. Here, the recent development of OCLP-enabled multifunctional microfluidic chips, including several accessible photochemical/photophysical schemes, and photosensitive materials permiting OCLP, is reviewed. To demonstrate the capability of OCLP technology, a series of typical micro-components fabricated using OCLP are introduced. The prospects and current challenges of this field are discussed. [ABSTRACT FROM AUTHOR]

We report herein the engineering of the surface/interface properties of graphene oxide (GO) films by controllable photoreduction treatment. In our recent works, typical photoreduction processes, including femtosecond laser direct writing (FsLDW), laser holographic lithography, and controllable UV irradiation, have been employed to make conductive reduced graphene oxide (RGO) microcircuits, hierarchical RGO micro-nanostructures with both superhydrophobicity and structural color, as well as moisture-responsive GO/RGO bilayer structures. Compared with other reduction protocols, for instance, chemical reduction and thermal annealing, the photoreduction strategy shows distinct advantages, such as mask-free patterning, chemical-free modification, controllable reduction degree, and environmentally friendly processing. These works indicate that the surface and interface engineering of GO through controllable photoreduction of GO holds great promise for the development of various graphene-based microdevices. [ABSTRACT FROM AUTHOR]

Inspired from butterfly wings that exhibit unique dewetting properties and brilliant structural color synchronously, we reported here the preparation of biomimetic few-layer graphene films through a template-directed chemical vapor deposition method using laser-structured Cu foil as substrates. Hierarchical micronanostructures, including microscale stripes derived from the laser scanning and nanoscale laser-induced periodic surface structures (LIPSS), formed on Cu foil after a simple femtosecond laser treatment. By tuning the laser power, the surface roughness of the resultant Cu foils can be well controlled. Using the laser structures Cu foil as templates, biomimetic few-layer graphene films with both iridescence and superhydrophobicity have been successfully prepared. The present work may open up a new way to design and prepare structured graphene film in a biomimetic manner, and we deem that the bioinspired few-layer graphene films may find broad applications in the near future. [ABSTRACT FROM AUTHOR]

Inspired by natural autonomous systems that demonstrate controllable shape, appearance, and actuation under external stimuli, a facile preparation of moisture responsive graphene-based smart actuators by unilateral UV irradiation of graphene oxide (GO) papers is reported. UV irradiation of GO is found to be an effective protocol to trigger the reduction of GO; however, due to the limited light transmittance and thermal relaxation, thick GO paper cannot be fully reduced. Consequently, by tuning the photoreduction gradient, anisotropic GO/reduced GO (RGO) bilayer structure can be easily prepared toward actuation application. To get better control over the responsive properties, GO/RGO bilayer paper with a certain curvature and RGO patterns are successfully prepared for actuator design. As representative examples, smart humidity-driven graphene actuators that mimic the cilia of respiratory tract and tendril climber plant are successfully developed for controllable objects transport. [ABSTRACT FROM AUTHOR]

Surface‐enhanced Raman spectroscopy (SERS) has been combined with microfluidic Lab‐on‐a‐Chip (LoC) systems for sensitive optofluidic detection for more than a decade. However, most microfluidic SERS devices still suffer from analyte contamination and signal irreproducibility. In recent years, both the microfluidics and SERS communities have developed their own solutions that are complementary to each other; their combination even has potential for commercialization. In this review, the recent advances in both fields are summarized with regard to the development of reliable multifunctional SERS‐enabled LoC systems and their broad applications. Starting from SERS fundamentals, reproducible SERS substrates and dynamic microfluidic trapping are discussed. Based on their combination, on‐chip applications beyond SERS are presented, and insight can be gained into the commercialization of portable SERS chips. [ABSTRACT FROM AUTHOR]

Reported here is a bioinspired fabrication of superhydrophobic graphene surfaces by means of two-beam laser interference (TBLI) treatment of graphene oxide (GO) films. Microscale grating-like structures with tunable periods and additional nanoscale roughness are readily created on graphene films due to laser induced ablation effect. Synchronously, abundant hydrophilic oxygen-containing groups (OCGs) on GO sheets can be drastically removed after TBLI treatment, which lower its surface energy significantly. The synergistic effect of micro-nanostructuring and the OCGs removal endows the resultant graphene films with unique superhydrophobicity. Additionally, dual TBLI treatment with 90° rotation is implemented to fabricate superhydrophobic graphene films with two-dimensional grating-like structures that can effectively avoid the anisotropic hydrophobicity originated from the grooved structures. Moreover, the superhydrophobic graphene films become conductive due to the laser reduction effect. Unique optical characteristics including transmission diffraction and brilliant structural color are also observed due to the presence of periodic microstructures. As a mask-free, chemical-free, and cost-effective method, the TBLI processing of GO may open up a new way to biomimetic graphene surfaces, and thus hold great promise for the development of novel graphene-based microdevices. [ABSTRACT FROM AUTHOR]

In view of mass‐production and solution‐processing capabilities, graphene oxides (GOs), generally prepared by chemical oxidation of graphite and subsequent exfoliation in aqueous solution, are widely used as an effective route to graphene‐like materials. However, the oxygen‐containing groups (OCGs) on the graphene sheets make GO insulating, which significantly restricts its applications, especially for electronics. Therefore, reduction methods that are used to remove OCGs become critical. In recent years, in addition to thermal and chemical reduction, photoreduction has emerged as an appealing alternative because photoreduction does not rely on either high temperature or toxic chemicals. In this progress report, the recent development of the photoreduction of GOs and their unique properties are highlighted, as well as their related applications. Photoreduction strategies including photothermal reduction, catalytic/catalyst‐free photochemical reduction, and solid state/in‐solution laser reduction are summarized. Moreover, photoreduction of GO permits exquisite control over film conductivities, residual oxygen contents, porosity, and surface wettability, which lead to various functionalities towards a wide range of applications, such as field‐effect‐transistors (FETs), flexible electrodes, sensors, supercapacitors, Li‐ion batteries, photovoltaic devices, and photocatalysis. It is anticipated that, with the rapid progress of photoreduction methodology, GOs would be more competitive in the graphene‐oriented applications. [ABSTRACT FROM AUTHOR]

Over the past two decades, microfluidics, represented by lab-on-a-chip (LoC) systems, have been developed because of their unique advantages of low reactant consumption, environmental friendliness, high safety, high efficiency, high sensitivity, portability, and easy handling of reactants. The distinguishing features of microfluidics have made the on-chip reactor a highly efficient platform for general chemical experiments, especially catalysis. In this paper, through a brief review of the recent work on microfluidic catalysis, we highlight the importance of on-chip catalytic microreactors. New approaches to the fabrication of on-chip catalytic microreactors and their integration with multifunctional components are briefly introduced. Finally, the current challenges and future perspectives of this up-and-coming field are discussed based on our own opinions. It is believed that, with the progress of interdisciplinary cooperation, microfluidics and catalysis could be complementary sciences; catalysts may play a very important role in LoC systems, and on-chip catalytic microreactors could be a highly efficient experimental platform for modern catalysis research. [ABSTRACT FROM AUTHOR]

Abstract: Reported here is the synthesis of pyridine-functionalized porous polymers, which are designed as homogeneous-like base catalysts. These highly porous catalysts have adjustable pyridine contents, high BET surface area (312–649m2/g), large pore volume (0.5–2.0cm3/g) and rapid swelling property, thus they efficiently combined the advantage of both homogeneous and heterogeneous catalysts. The exposure degree of active sites in our homogeneous-like catalysts has been evaluated by Cu2+ adsorption, giving similar capacity with homogeneously dissolved poly-4-vinylpyridine. In the Knoevenagel condensation, these materials exhibit excellent activity and stability compared with Mg–Al hydrotalcite and magnesia as well as homogeneous base catalyst of poly-4-vinylpyridine. [Copyright &y& Elsevier]

Abstract: Reported in this paper is solvothermal fabrication of nanoporous polymer monolith for biomolecules adsorption. General functional groups such as carboxyl and amido could be easily introduced into the nanoporous polymers by in situ polymerization of divinylbenzene and the monomers of methacrylic acid or acrylamide. The synthesized polymers exhibit high BET surface areas (105–499m2/g), large pore volumes (0.41–1.22cm3/g), and large pore size (10–100nm), which were quite suitable for biomolecules adsorption. As representative tests, myoglobin was chosen as a target adsorbate, and all these nanoporous polymers show much higher adsorptive capacities than conventional materials such as commercial resin (XAD-4) and activated carbon. Our nanoporous polymer monolith would be potentially important for enzyme immobilization. [Copyright &y& Elsevier]

Soft robots controlled by different actuation schemes are flourishing owing to the continued development of smart materials. However, most of the existing actuators are powered by a single source with predetermined mechanical properties and motion characteristics. Speed, power, and efficiency of these actuators are thus far inferior to their conventional counter parts. How to preload or alter the internal energy distribution and trigger rapid kinetic energy release combined with re‐programmability is a challenge and corresponding solutions will extend the practical use of soft robotics. Herein, a hybrid magnetically and photothermally responsive actuator with high degrees of freedom by using a coupled‐field manipulation strategy is proposed. As a proof‐of‐concept, a crab robot (CraBot) that contains uniformly distributed superparamagnetic particles and localized light‐responsive joints is produced. The spatial magnetic field exerts force on the robot, leading to real‐time adjustment of energy distribution within the entire robot. Meanwhile, the focused light field enables selective deformation of specific joints, releasing the accumulated energy into kinetic energy of motion for quick actuation. The directional accumulation and addressable release of elastic energy enables the CraBot to walk efficiently with improved power and speed. Such a hybrid‐field manipulation strategy holds great promise for sophisticated actuation of soft robots. [ABSTRACT FROM AUTHOR]

MXene, which is known for its high electrical/thermal conductivity, surface hydrophilicity, excellent mechanical flexibility, and chemical stability, is a versatile and smart material for soft actuators. However, most MXene actuators are fabricated by combining MXene with other inert materials to form a bilayer or multilayer structure. Considering the strain mismatch at multimaterial interfaces under frequent deformation, MXene‐based actuators are generally associated with poor stability, which limits their practical applications. Herein, inspired by the natural quantum‐confined superfluidic (QSF) effect, a multiresponsive MXene actuator that can be driven by moisture, light, and electricity by engineering an asymmetric QSF structure on both sides of the MXene film is reported. The actuation mechanism of the MXene film can be attributed to nonuniform water adsorption, transport, and desorption within the asymmetric QSF channels under moisture, photothermal, and electrothermal stimuli. Interestingly, MXene actuators can be flexibly formed into various shapes under moisture‐assisted mechanical compression, which not only enhances their multiresponsive actuation, but also permits a more complex deformation. As proof‐of‐concept demonstrations, various intriguing applications including a dual‐role robot, a smart shielding curtain, and a dragonfly robot, are fabricated, revealing the potential of MXene actuators for soft robotics. [ABSTRACT FROM AUTHOR]

In pursuit of versatile microfluidic chips fabrication, flexible integration of multifunctional components within a tiny chip is still challenging because the non‐flat micro‐channels of microfluidic chips make it impossible to fabricate devices using conventional 2D processing technologies, such as, lithography and nanoimprinting. Recently, on‐chip laser processing (OCLP) technology has emerged as an appealing alternative for achieving chip functionalization by in situ fabrication of 3D microstructures. In this cover, the authors highlight the contribution of OCLP to chip functionalization, as a series of typical micro‐devices, represented by the micro‐turbine and the letters “d, e, v, i, c, e, s” have been integrated at the key position of a microfluidic chip (the intersection of two channels). (Picture: Huan Wang et al., article number 1600116, in this issue) [ABSTRACT FROM AUTHOR]

Inspired from butterfly wings that feature brilliant structural color and unique dewetting properties, micro‐nanostructured graphene surfaces with superhydrophobicity and iridescence are fabricated on page 4595 by Y.‐L. Zhang, H.‐B. Sun, and co‐workers using a two‐beam laser interference treatment of graphene oxide films. As a mask‐free, chemical‐free, highly efficient and cost‐effective method, two‐beam laser interference treatment processing of GO may open up a new way to biomimetic graphene surfaces, and thus hold great promise for the development of novel graphenebased microdevices. [ABSTRACT FROM AUTHOR]

Abstract: Flexible smart surfaces with tunable wettability are promising for emerging wearable uses. However, currently, wearable superhydrophobic surfaces with dynamic wetting behaviors are rarely reported. Here, a skin‐like superhydrophobic elastomer surface with switchable lotus leaf and rose petal states is reported. Direct laser writing technique is employed for one‐step, programmable, large‐scale fabrication of monolithic and hierarchical micro‐nanostructures on elastomer, leading to strong water repellence. The surface topography can be finely regulated in a rapid and reversible manner by simple stretching, providing the feasibility of controlling the surface wettability by simple body motions. The ability to switch wetting states enables the surface to capture and release multiple droplets in parallel. Furthermore, the active surface can be applied to the joints of fingers and operate as a droplet manipulator under finger motions without requiring energy supply or external appliance. In this work, dynamic tuning of wetting properties is integrated into the design of skin‐like wearable surfaces, revealing great potential in versatile applications such as wearable droplet manipulator, portable actuator, adaptive adhesion control, liquid repellent skin, and smart clothing. [ABSTRACT FROM AUTHOR]

Recent advances in developing soft electronic devices have increased the demand for deformable storage devices. However, the fabrication of microsupercapacitors (MSCs) with satisfactory electrochemical performance and mechanical robustness remains a crucial challenge. In this work, deformable moisture-activated all-solid-state planar MSCs were designed and fabricated by an in situ laser reduction technology. The planar MSC shows a high areal-specific capacitance (∼4.7 mF cm−2 at 5 mV s−1) under high moisture (RH = 100%). Moreover, the tensile strength of the deformable planar MSC increased to 21 MPa. Moreover, the mechanical robustness of the planar MSC allows them to be folded into origami. The deformable moisture-activated all-solid-state planar MSC holds promises for soft storage devices. [ABSTRACT FROM AUTHOR]

Chemical Marangoni propulsion enables dynamic and untethered motion by generating surface tension gradient through chemical release, thereby having great potential for the development of insect‐scale self‐propelled robots. However, as the release and diffusion of chemical "fuels" are commonly uncontrollable, the Marangoni propulsion is unstable, thereby restricting robotic applications. Herein, the laser fabrication of superhydrophobic swimming robots to develop controllable Marangoni propulsion based on a photothermal composite of graphene and polydimethylsiloxane is reported. By combining the microfluidic channels with photothermal air chambers, a light‐triggered switch that can control the release of chemical "fuels" is proposed. Furthermore, a superhydrophobic surface is fabricated on the swimming robot by laser treatment, which reduced water resistance and promoted propulsion. On‐demand actuation and swimming route planning are realized by programming the alcohol/air segments in the releasing channels, on‐demand actuation and swimming route planning have been realized. As a proof‐of‐concept, a Marangoni swimming robot equipped with a miniature digital camera is used in an actual environment. Therefore, this study is expected to advance the practical applications of the chemical Marangoni effect in swimming robots. [ABSTRACT FROM AUTHOR]

Review: 103 refs. [ABSTRACT FROM AUTHOR]

[Display omitted] Photothermal responsive slippery surfaces with switchable superwettability are promising in the fields of biomedicine, self-cleaning, anti-corrosion, and lab-on-a-chip systems. However, the development of a light switchable slippery surface that combines high-performance photothermal materials with hierarchical microstructures of special orientation remains challenging, which limits the applications in anisotropic droplet manipulation. Herein, we demonstrate a photothermal responsive slippery surface based on laser-structured graphene and polyvinylidene difluoride composites (L-G@PVDF) for controllable droplet manipulation. The L-G@PVDF film exhibits high light absorption (∼95.4%) in the visible and NIR region. After lubricating with paraffin, the resultant surface shows excellent self-healing ability and light-responsive wettability change due to the photothermal effect of L-G@PVDF and the hot melting effect of paraffin. Additionally, by introducing anisotropic grooved structures, the paraffin-infused L-G@PVDF surface displays anisotropic wettability that further affects droplet manipulation under light irradiation. Also, the photothermal responsive slippery property endows the paraffin-infused L-G@PVDF surface with excellent anti-frosting and de-icing capability. Moreover, the smart paraffin-infused L-G@PVDF surface can be combined with a microfluidics chip for light-driven automatic sampling. This study offers insight into the rational design of photothermal responsive slippery surfaces for controllable droplet manipulation. [ABSTRACT FROM AUTHOR]

Graphene oxide (GO), which has many oxygen functional groups, is a promising candidate for use in moisture‐responsive sensors and actuators due to the strong water–GO interaction and the ultrafast transport of water molecules within the stacked GO sheets. In the last 5 years, moisture‐responsive actuators based on GO have shown distinct advantages over other stimuli‐responsive materials and devices. Particularly, inspired by nature organisms, various moisture‐enabled soft robots have been successfully developed via rational assembly of the GO‐based actuators. Herein, the milestones in the development of moisture‐responsive soft robots based on GO are summarized. In addition, the working mechanisms, design principles, current achievement, and prospects are also comprehensively reviewed. In particular, the GO‐based soft robots are at the forefront of the advancement of automatable smart devices. [ABSTRACT FROM AUTHOR]

Graphene oxide (GO), which has many oxygen functional groups, is a promising candidate for use in moisture‐responsive sensors and actuators due to the strong water–GO interaction and the ultrafast transport of water molecules within the stacked GO sheets. In the last 5 years, moisture‐responsive actuators based on GO have shown distinct advantages over other stimuli‐responsive materials and devices. Particularly, inspired by nature organisms, various moisture‐enabled soft robots have been successfully developed via rational assembly of the GO‐based actuators. Herein, the milestones in the development of moisture‐responsive soft robots based on GO are summarized. In addition, the working mechanisms, design principles, current achievement, and prospects are also comprehensively reviewed. In particular, the GO‐based soft robots are at the forefront of the advancement of automatable smart devices. [ABSTRACT FROM AUTHOR]

Photoreduction of graphene oxide (GO) holds great potential for developing graphene-based electrodes for high-performance supercapacitors (SCs). However, the insufficient micro-nanostructure on photoreduced GO (PRGO) restricts its electrochemical performance. Here, a hierarchically structured PRGO-based planar SC is reported by combining two-beam-laser-interference with the masking technique. The hierarchical structures improve the surface area between PRGO and electrolyte and contribute to format electric double-layer capacitors. Planar device structures with PRGO-based interdigital finger current collectors are beneficial for rapid ion diffusion paths. As a result, the hierarchically structured PRGO-based planar SC achieves an areal capacitance of 3.97 mF cm−2 at 10 mV s−1. The proposed strategy of employing hierarchically structured PRGO in the planar SC design offers a new route for manufacturing high-performance integrated energy storage devices. [ABSTRACT FROM AUTHOR]

Direct light‐to‐work conversion enables remote actuation through a non‐contact manner, among which the photothermal Marangoni effect is significant for developing light‐driven robots because of the diversity of applicable photothermal materials and light sources, as well as the high energy conversion efficiency. However, the lack of nanotechnologies that enable flexible integration of advanced photothermal materials with actuators of complex configurations significantly restricts their practical applications. In this paper, laser‐induced graphene (LIG) tape is reported as stick‐on photothermal labels for developing light‐driven actuators based on the Marangoni effect. With the help of direct laser writing technology, graphene patterns with superior photothermal properties are prepared on the PI tape. The patterned LIG tape can be stuck on any desired objects and generates an asymmetric photothermal field under light irradiation, forming a photothermal Marangoni actuator. Additionally, the PI tape with LIG patterns can be folded into 3D origami actuators that permit photothermal Marangoni actuation including both translation and rotation. The graphene‐based photothermal Marangoni actuators feature biocompatibility, which is confirmed by MDA‐MB‐231 cells proliferation experiments. Owing to the excellent photothermal property of LIG patterns, the as‐produced photothermal actuators can be manipulated by a variety of light sources, holding great promise for developing light‐driven soft robots. [ABSTRACT FROM AUTHOR]

Stimuli-Responsive Materials: Smart Compound Eyes Enable Tunable Imaging (Adv. Funct. Keywords: compound eyes; femtosecond laser; smart materials; tunable optical components; variable-focus imaging Compound eyes, femtosecond laser, smart materials, tunable optical components, variable-focus imaging. [Extracted from the article]

Compound eyes are natural multiaperture optical imaging systems and have substantial potential in the field of modern optics. However, both natural and artificial compound eyes are composed of ommatidia with fixed focal lengths, and thus incapable of variable‐focus imaging. In this study, inspired by the tunable crystalline lens of human eyes, smart stimuli‐responsive compound eyes based on the bovine serum album (BSA) protein are fabricated via femtosecond laser direct writing. Due to the swelling and shrinking effect of BSA under different pH conditions, a tunable field of view (FOV, 35°–80°) and variable focal length of ommatidia are achieved. In addition to the direct prototyping of an entire protein‐based compound eye, the ability to flexibly integrate the smart protein ommatidia with a conventional optical lens (an SU‐8 lens in this study) to form a composite compound eye is shown. The composite compound eye achieves nearly 400% of focal length tuning at a fixed FOV. It is anticipated that femtosecond laser fabrication and the integration of smart protein‐based compound eyes may emerge as an enabler for fabricating miniature tunable imaging systems. [ABSTRACT FROM AUTHOR]

Graphical abstract Highlights • Direct laser writing treatment of In 2 O 3 @GO composite could lead to the reduction of GO and the formation of a porous structure. • Complex patterns of In 2 O 3 @RGO could be fabricated through a programmable manner by direct laser writing technology. • NO 2 sensors arrays could be fabricated on flexible substrates, which can be operated at room temperature. • NO 2 sensors based on In 2 O 3 @RGO show liner NO 2 sensing properties, good response/recovery feature and excellent selectivity towards NO 2. Abstract In this work, we reported the fabrication of flexible NO 2 sensors arrays operating at room temperature on a composite film of In 2 O 3 and graphene oxide (GO) by direct laser writing (DLW) technology. The laser treatment not only induced the photoreduction of GO, leading to a highly porous structure due to the removal of oxygen groups, but also permitted mask-free patterning through a programmable manner, enabling flexible integration of sensor arrays on any substrates. We demonstrated the fabrication of a 2 × 4 NO 2 sensors array on a flexible polyimide substrate within 10 min. Our NO 2 sensors based on In 2 O 3 and reduced GO (In 2 O 3 @RGO) show liner NO 2 sensing properties at room temperature, good responsivity and recovery properties, as well as excellent selectivity towards NO 2. We deem that the DLW fabrication of flexible NO 2 sensorsarrays may contribute to the development of flexible electronics. [ABSTRACT FROM AUTHOR]

Direct light-to-work conversion enables manipulating remote devices in a contactless, controllable, and continuous manner. Although some pioneering works have already proven the feasibility of controlling devices through light-irradiation-induced surface tension gradients, challenges remain, including the flexible integration of efficient photothermal materials, multifunctional structure design, and fluidic drag reduction. This paper reports a facile one-step method for preparing light-driven floating devices with functional surfaces for both light absorption and drag reduction. The direct laser writing technique is employed for both arbitrary patterning and surface modification. By integrating the functional layer at the desired position or by designing asymmetric structures, three typical light-driven floating devices with fast linear or rotational motions are demonstrated. Furthermore, these devices can be driven by a variety of light sources including sunlight, a filament lamp, or laser beams. The approach provides a simple, green, and cost-effective strategy for building functional floating devices and smart light-driven actuators. [ABSTRACT FROM AUTHOR]

We report here a facile preparation of graphene quantum dots (GQDs) by chemical exfoliation of multiwall carbon nanotubes (MWCNTs) using a modified hummers' method. The resultant GQD samples possess strong electronic property, revealing great potential for photocatalyst design. As an efficient promoter, GQDs/P25 nanocomposites have been successfully prepared by simple wet impregnation and subsequent thermal annealing at 200 °C. In the tests of photocatalytic degradation of organic dyes under visible-light irradiation, the GQDs promoted P25 samples which shows much higher photocatalytic activity compared to the pure P25, indicating the crucial roles of GQDs. [ABSTRACT FROM AUTHOR]

We report controllable assembly of silver nanoparticles (Ag NPs) for patterning of silver microstructures. The assembly is induced by femtosecond laser direct writing (FsLDW). A tightly focused femtosecond laser beam is capable of trapping and driving Ag NPs to form desired micropatterns with a high resolution of ∼190 nm. Taking advantage of the ‘direct writing’ feature, three microelectrodes have been integrated with a microfluidic chip; two silver-based microdevices including a microheater and a catalytic reactor have been fabricated inside a microfluidic channel for chip functionalization. The FsLDW-induced programmable assembly of Ag NPs may open up a new way to the designable patterning of silver microstructures toward flexible fabrication and integration of functional devices. [ABSTRACT FROM AUTHOR]

• Recent advances in laser-induced color centers in different crystals are comprehensively reviewed, including diamond, silicon carbide, alkali halide crystals and others. • Cutting-edge applications of laser-induced color centers are introduced. • Current challenges and future perspective of this field have been discussed. • Cited figures are adapted carefully for a better understanding for readers. Color centers are widely used in quantum information, quantum sensing, micro-nano optics and other relevant fields. In addition to the traditional ways that can generate color centers, for instance, ion beam implantation, direct laser writing (DLW) technology has recently emerged as an appealing alternative to induce color centers because it enables true three-dimensional and high precision machining. Particularly, DLW can induce color centers near/on the surface or inside the crystals with a homogeneous and pure surrounding environment, which permits subsequent integration with other components. In this paper, the recent advances in laser-induced color centers in different crystals are comprehensively reviewed, including diamond, silicon carbide, alkali halide crystals and others. Meanwhile, cutting-edge applications of laser-induced color centers are introduced. Lastly, current challenges and future perspective of this field have been discussed. [ABSTRACT FROM AUTHOR]

Graphene quantum dots (GQDs) have recently emerged as a promising type of low‐toxicity, high‐biocompatibility, and chemically inert fluorescence probe with a high resistance to photobleaching. They are a prospective substitution for organic materials in light‐emitting devices (LED), enabling the predicted concept of much brighter and more robust carbon LED (CLED). However, the mechanism of GQD emission remains an open problem despite extensive studies conducted so far, which is becoming the greatest obstacle in the route of technical improvement of GQD quantum efficiency. This problem is solved by the combined usage of femtosecond transient absorption spectroscopy and femtosecond time‐resolved fluorescence dynamics measured by a fluorescence upconversion technique, as well as a nanosecond time‐correlated single‐photon counting technique. A fluorescence emission‐associated dark intrinsic state due to the quantum confinement of in‐plane functional groups is found in green‐fluorescence graphene quantum dots by the ultrafast dynamics study, and the two characteristic fluorescence peaks that appear in all samples are attributed to independent molecule‐like states. This finding establishes the correlation between the quantum confinement effect and molecule‐like emission in the unique green‐fluorescence graphene quantum dots, and may lead to innovative technologies of GQD fluorescence enhancement, as well as its broad industrial application. [ABSTRACT FROM AUTHOR]

Abstract: First-principles calculation identifies elementary processes in the thermal reduction of graphene oxide (GO) and reveals the effects of alkaline-earth metals (AEMs) in recovering the graphene. These metals are highly effective in removing residual oxygen groups resistive to thermal reduction, as well as healing the defects formed during the reduction, such as the carbonyl groups. In the AEM-assisted reduction, the AEMs serve as an electron reservoir of high chemical potential that forces electron transfer to the GO, whereas pristine carbon regions on the GO serve as a “bridge” to facilitate the electron transfer directly to oxidized carbon. This enables fast kinetics for the breaking of both C–O and CComplete reduction is observed in our simulation at T ≤600K within 32ps for a 28%-oxygen-coverage GO model. [Copyright &y& Elsevier]

Abstract: Reported in this paper is a solvothermal synthesis of highly porous polydivinylbenzene. The nanoporous structures of the resultant polymers could be modulated from macro/mesoporosity to meso/microporosity by simply changing the amount of acetone solvent in the synthesis. A micro-phase separation during the solvothermal process was found to be the key factor for this transition in porous structures. The hierarchically porous polymers prepared here were characterized by N2 physi-sorption, scanning electron microscopy (SEM), transmission electron microscopy (TEM), and contact angle testing. Experimental results show that these nanoporous polymers have large BET surface areas (up to 420m2/g), large pore volumes (up to 1.73cm3/g), and superhydrophobicity due to their highly porous structures, which make these nanoporous materials an excellent candidate for selective removal of toxic volatile organic compounds (VOCs). In the adsorption tests, the nanoporous polymers show outstanding adsorptive capacity and very high selectivity to organic compounds, giving a great potential for indoor VOCs removal. [Copyright &y& Elsevier]

Abstract: Two-beam-laser interference was used for the simultaneous reduction, patterning and nanostructuring of graphene oxide on flexible polyethylene terephthalate substrates for the production of a high performance humidity sensing device. Hierarchical graphene nanostructures were formed after laser interference treatment of graphene oxide, which holds great promise for gaseous molecular adsorption, and thereby significantly increases their sensing performance. By tuning the laser power, the content of oxygen functional groups, could be changed within a certain range, which contributes not only controllable conductivity but also tunable response/recovery time of the humidity sensor due to the interaction between water molecules and oxygen functional groups on the graphene oxide sheets. The laser interference processing of graphene oxide films is a mask-free, surfactant-free and large-area approach to the production of hierarchical graphene micro-nanostructures, and thus shows great potential for fabrication of future graphene-based microdevices. [Copyright &y& Elsevier]

The rapid progress of microfluidics has contributed to modern analytical methodology. However, in situ integration of chemical/biological sensors for on‐chip reaction monitoring remains a big challenge. Herein, reported is the fabrication of an integrated surface‐enhanced Raman scattering (SERS) sensor and graphene‐based catalytic chip by laser scribing of graphene oxide (GO) and Ag nanoparticles (AgNPs) composite (AgNPs@GO). The surface plasmonic effect of AgNPs can promote the photoreduction of GO, inducing a high porous nanostructure. By combining the AgNPs@RGO nanocomposite patterns with polydimethylsiloxane microfluidic channels, a bi‐functional microfluidic chip capable of on‐chip catalysis and SERS detection is fabricated. As a proof‐of‐concept demonstration, on‐chip AgNPs‐catalyzed 4‐nitrophenol (4‐NP) reduction has been implemented, in which the reaction process can be well monitored using the in situ SERS sensor. The integration of SERS sensors with functional microfluidic devices may hold great promise for developing advanced Lab‐on‐a‐Chip systems. [ABSTRACT FROM AUTHOR]

Graphene oxide (GO) with tunable physical/chemical properties is a versatile material for smart bimorph actuators. Using GO or its derivatives (e.g., reduced GO, RGO) as an active material, actuators can be manipulated under various external stimuli including moisture, light, temperature, and electricity. However, most of these GO‐based actuators respond to a solo stimulus, which limits its cutting‐edge applications in soft robotics. Here, the programmable patterning of RGO/GO Janus paper using a threshold‐controlled direct laser writing (DLW) technology is reported. By combining the RGO/GO Janus paper with a common thermally expansive polymer layer, a moisture, light, and electricity multiresponsive actuator is fabricated, in which the RGO interlayer plays multiroles including moisture‐passive layer, photothermal/electrothermal layer, thermal conductive layer, and inert layer for thermal expansion. As a proof of concept, multiresponsive actuators including a bidirectional cantilever and a smart curtain are fabricated, demonstrating the great potential for developing soft robots. [ABSTRACT FROM AUTHOR]

With high thermal and mechanical stability, glass artificial compound eyes have great potential applications in wide field‐of‐view (FOV) imaging and fast detection. However, the rapid fabrication of large‐area, high integration, uniform, and well‐designed three‐dimensional (3D) glass compound eyes is still a great challenge. Here, a dry‐etching‐assisted femtosecond laser machining (DE‐FsLM) technology is proposed for fabrication of cm‐sized concave compound eye from a curved sapphire substrate, with which the fabrication efficiency can be improved by over two orders of magnitude compared with direct laser ablation. With high hardness and thermal stabilities, the sapphire concave compound eyes can be used as high‐temperature and hard‐casting templates for the replication of convex compound eyes on K9 glass. The replicated cm2‐size all‐glass compound eye consists of a spherical macrolens (1 cm diameter and 2.3 mm height) and over 190 000 close‐packed ommatidia (≈20 µm diameter and 1.5 µm height). The compound eyes exhibit excellent optical properties with wide FOV (up to 90°) imaging and focusing. These results indicate that the DE‐FsLM and casting replication technology will open new opportunities in micro‐/nanofabrication of hard materials. [ABSTRACT FROM AUTHOR]

The strong interaction between water molecules and graphene oxide (GO) enables moisture‐responsive graphene actuators, revealing great potential for soft robots. However, current strategies for developing smart graphene actuators fail to tailor their material property gradient in a controlled manner, and the driving manner is usually limited to single stimulus actuation. Here, a facile preparation of humidity/thermal/light multiresponsive graphene actuators by sequential vacuum filtration of GO and reduced GO (RGO) aqueous solutions is reported. The photoreduction degree of RGO layer is tuned precisely beforehand by changing ultraviolet (UV) light irradiation time, and thus a pretailored reduction gradient along the normal direction of the GO/RGO bilayer paper would form in a highly controlled manner. Taking advantage of the competitive water adsorption between the GO and RGO layers, as well as the thermal‐, light‐promoted desorption, the GO/RGO bilayers deform in response to moisture, light, and temperature changes; and the deformation degree can be modulated by controlling the gradient of oxygen‐containing groups (OCGs). As a proof of principle, a humidity‐responsive graphene mimosa and a humidity/thermal/light multiresponsive graphene actuators are fabricated. The GO/RGO bilayer paper with pretailored reduction gradient holds great promise for easy fabrication of biomimetic actuators that enable performing predictable deformation. Humidity/thermal/light multiresponsive graphene actuators are prepared by sequential vacuum filtration of graphene oxide (GO) and reduced GO (RGO) with a pretailored reduction gradient. GO/RGO bilayer actuators with tunable curving performance are achieved by controlling the photoreduction degree. Humidity responsive mimosa and multiresponsive paper robot are designed based on the competitive water adsorption between GO/RGO layers and the thermal‐, light‐promoted water desorption. [ABSTRACT FROM AUTHOR]