Temperature-Regulated Bidirectional Capillary Force Self-Assembly of Femtosecond Laser Printed Micropillars for Switchable Chiral Microstructures.

Bottom-up self-assembly is regarded as an alternative way to manufacture series of microstructures in many fields, especially chiral microstructures, which attract tremendous attention because of their optical micromanipulations and chiroptical spectroscopies. However, most of the self-assembled microstructures cannot be tuned after processing, which largely hinders their broad applications. Here, we demonstrate a promising manufacturing strategy for switchable microstructures by combining the flexibility of femtosecond laser printing induced capillary force self-assembly and the temperature-responsive characteristics of smart hydrogels. Through designing asymmetric cross-link density, the printed microarchitectures can be deformed in the opposite direction and assembled into switchable ordered microstructures driven by capillary forces under different temperatures. Finally, the assembled chiral microstructures with switchable opposite handedness are realized, which shows tunable vortical dichroism. The proposed strategy holds potential applications in the fields of chiral photonics, chiral sensing, and so on.

Overcoming Long-Range Unidirectional Transport of Underwater Bubbles on Laser-Textured Single-Layer Superaerophobic Dual-Rail Arrays.

Understanding the behavior of gas bubbles in aqueous media has been a hot topic because of their vital roles in both scientific research and industrial applications. Wettability gradient force and Laplace pressure are two typical characteristics of bubble transport. However, most work about bubble transport is limited to a short distance. Therefore, we took inspiration from the structure of the Nepenthes pitcher and prepared superaerophobic dual-rail arrays (SDRA). Upon SDRA, with this structure of a uniform distribution of superaerophobic and superaerophilic zones, bubbles can be transported over long distances on the structure's surface. The underlying principle is that gas bubbles tend to spread out on the superaerophilic region until they make contact with the asymmetric superaerophobic barriers. An asymmetric spreading resistance force is generated, which is attributed to the different lengths of the three-phase contact line (TCL) between gas bubbles and superaerophobic barriers. In addition, diverse parameters are quantified to investigate the critical transport state between unidirection and bidirection. Under the function of SDRA, the structure surface can realize bubble collection. The transporter as well as the light-control-light shutter is also successfully deployed. The present study will inspire people to develop innovative strategies to effectively manipulate gas bubbles in practical applications.

Multiple-Droplet Selective Manipulation Enabled by Laser-Textured Hydrophobic Magnetism-Responsive Slanted Micropillar Arrays with an Ultrafast Reconfiguration Rate.

Biomimetic structures based on the magnetic response have attracted ever-increasing attention in droplet manipulation. Till now, most methods for droplet manipulation by a magnetic response are only applicable to a single droplet. It is still a challenge to achieve on-demand and precise control of multiple droplets (≥2). In this paper, a strategy for on-demand manipulation of multiple droplets based on magnetism-responsive slanted micropillar arrays (MSMAs) is proposed. The Glaco-modified superhydrophobic surface is the basis of multiple-droplet manipulation. The droplet's motion mode (pinned, unidirectional, and bidirectional) can be readily fine-tuned by changing the volume of droplets and the speed of the magnetic field. The rapid movement of droplets (10-80 mm/s) in the horizontal direction is realized by the unidirectional waves of the micropillar array driven by a specific magnetic field. The bending angle of micropillars can be rapidly and reversibly adjusted from 0 to 90° under the action of a magnetic field. Meanwhile, the liquid-involved light, electric switch, and biomedical detection can be designed by manipulating the droplets on demand. The superiority of MSMAs in multiple-droplet programmable manipulation opens up an avenue for applications in microfluidic and biomedical engineering.

Tethered and Untethered 3D Microactuators Fabricated by Two-Photon Polymerization: A Review.

Microactuators, which can transform external stimuli into mechanical motion at microscale, have attracted extensive attention because they can be used to construct microelectromechanical systems (MEMS) and/or microrobots, resulting in extensive applications in a large number of fields such as noninvasive surgery, targeted delivery, and biomedical machines. In contrast to classical 2D MEMS devices, 3D microactuators provide a new platform for the research of stimuli-responsive functional devices. However, traditional planar processing techniques based on photolithography are inadequate in the construction of 3D microstructures. To solve this issue, researchers have proposed many strategies, among which 3D laser printing is becoming a prospective technique to create smart devices at the microscale because of its versatility, adjustability, and flexibility. Here, we review the recent progress in stimulus-responsive 3D microactuators fabricated with 3D laser printing depending on different stimuli. Then, an outlook of the design, fabrication, control, and applications of 3D laser-printed microactuators is propounded with the goal of providing a reference for related research.

Controllable double-helical microstructures by photonic orbital angular momentum for chiroptical response.

Three-dimensional helical microstructures are abundant in nature and can be applied as chiral metamaterials for advanced nanophotonics. Here we report a flexible method to fabricate double-helical microstructures with single exposure by recording the chirality of incident optical vortices. Two coaxial optical vortices can interfere to generate a helical optical field, confirmed by the numerical simulation. The diameters of double-helical microstructures can be tailored by the magnitude of topological charges. This fast manufacturing strategy provides the opportunity to efficiently yield helical microstructures. Finally, the chirality of double-helical microstructures can be reversibly read by optical vortices, demonstrating a strong chiroptical response.

Giant Helical Dichroism of Single Chiral Nanostructures with Photonic Orbital Angular Momentum.

Optical activity, demonstrating the chiral light-matter interaction, has attracted tremendous attention in both fundamental theoretical research and advanced applications of high-efficiency enantioselective sensing and next-generation chiroptical spectroscopic techniques. However, conventional chiroptical responses are normally limited in large assemblies of chiral materials by circularly polarized light, exhibiting extremely weak chiroptical signals in a single chiral nanostructure. Here, we demonstrate that an alternative chiral freedom of light-orbital angular momentum-can be utilized for generating strong helical dichroism in single chiral nanostructures. The helical dichroism by monochromatic vortex beams can unambiguously distinguish the intrinsic chirality of nanostructures, in an excellent agreement with theoretical predictions. The single planar-chiral nanostructure can exhibit giant helical dichroism of ∼20% at the visible wavelength. The vortex-dependent helical dichroism, expanding to single nanostructures and two-dimensional space, has implications for high-efficiency chiroptical detection of planar-chiral nanostructures in chiral optics and nanophotonic systems.

Gigantic vortical differential scattering as a monochromatic probe for multiscale chiral structures.

Spin angular momentum of light is vital to investigate enantiomers characterized by circular dichroism (CD), widely adopted in biology, chemistry, and material science. However, to discriminate chiral materials with multiscale features, CD spectroscopy normally requires wavelength-swept laser sources as well as wavelength-specific optical accessories. Here, we experimentally demonstrate an orbital-angular-momentum-assisted approach to yield chiroptical signals with monochromatic light. The gigantic vortical differential scattering (VDS) of ∼120% is achieved on intrinsically chiral microstructures fabricated by femtosecond laser. The VDS measurements can robustly generate chiroptical properties on microstructures with varying geometric features (e.g., diameters and helical pitches) and detect chiral molecules with high sensitivity. This VDS scheme lays a paradigm-shift pavement toward efficiently chiroptical discrimination of multiscale chiral structures with photonic orbital angular momentum. It simplifies and complements the conventional CD spectroscopy, opening possibilities for measuring weak optical chirality, especially on mesoscale chiral architectures and macromolecules.

Self-assembled micropillars fabricated by holographic femtosecond multi-foci beams forin situ trapping of microparticles.

Dynamic self-assembly of micropillars has found wide applications in targeted trapping, micro-crystallization and plasmonic sensing. Yet the efficient fabrication of micropillars array with high flexibility still remains a grand challenge. In this Letter, holographic femtosecond laser multi-foci beams (fs-MFBs) based on a spatial light modulator (SLM) is adopted to efficiently create micropillars array with controllable geometry and spatial distribution by predesigning the computer-generated holograms (CGHs). Based on these micropillars array, diverse hierarchical assemblies are formed under the evaporation-induced capillary force. Moreover, taking advantage of the excellent flexibility and controllability of fs-MFBs, on-demand one-bead-to-one-trap of targeted microspheres at arbitrary position is demonstrated with unprecedentedly high capture efficiency, unfolding their potential applications in the fields of microfluidics and biomedical engineering.

Chiral Assemblies of Laser-Printed Micropillars Directed by Asymmetrical Capillary Force.

Artificial microstructures composed of chiral building blocks are of great significance in the fields of optics and mechanics. Here, it is shown that highly ordered chiral structures can be spontaneously assembled by a meniscus-directed capillary force arising in an evaporating liquid. The chirality is facilitated by rationally breaking the intrinsic symmetry in the unit cells through cooperative control of the geometry and spatial topology of the micropillars. The interfacial dynamics of the assembly process are studied to show that the sequential self-organization of the micropillars is influenced by the geometries, stiffness, and spatial arrangements. A diversity of chiral assemblies with controlled handedness is yielded by varying the pillar number, height, cross-section, laser power, and spatial topology. Lastly, the differential reflectance of light carrying opposite orbital angular momentums on the assembled chiral architectures are investigated, showcasing their potential in the field of chiral photonics concerning enantioselective response and exceptional optical functions.

Mechanical-Tunable Capillary-Force-Driven Self-Assembled Hierarchical Structures on Soft Substrate.

Capillary-force-driven self-assembly (CFSA) has been combined with many top-down fabrication methods to be alternatives to conventional single micro/nano manufacturing techniques for constructing complicated micro/nanostructures. However, most CFSA structures are fabricated on a rigid substrate, and little attention is paid to the tuning of CFSA, which means that the pattern of structures cannot be regulated once they are manufactured. Here, by combining femtosecond laser direct writing with CFSA, a flexible method is proposed to fabricate self-assembled hierarchical structures on a soft substrate. Then, the tuning of the self-assembly process is realized with a mechanical-stretching strategy. With this method, different patterns of tunable self-assembled structures are obtained before tuning and after release, which is difficult to achieve with other techniques. In addition, as a proof-of-concept application, this mechanical tunable self-assembly of microstructures on a soft substrate is used for smart displays and versatile micro-object trapping.

Microtubes with Complex Cross Section Fabricated by C-Shaped Bessel Laser Beam for Mimicking Stomata That Opens and Closes Rapidly.

This article presents a new method for fabricating complex cross-sectional microtubes with a high aspect ratio at micro/nanoscale. The microtubes are directly written in a photoresist using a femtosecond pulsed laser combined with a spatial light modulator (SLM). A new method for generating a C-shaped Bessel beam by modifying the Bessel beams with a SLM is reported for the first time. Using this gap-ring-shaped light field, microtubes with special cross section (trefoil-shaped, clover-shaped, spiral, etc.) have been first achieved through two-photo polymerization rapidly. The microtube wall can reach about 800 nm and the diameter of the gap-ring structure is only a few micrometers. As a demonstration, artificial stomata were manufactured with the same size as actual plants stomata consisting of gap-ring microtubes. This artificial stomata can mimic the function of the real stomata with rapid opening and closing, demonstrating its ability to trap and release microparticles regulated by rinse solvent.

Generation of colorful Airy beams and Airy imaging of letters via two-photon processed cubic phase plates.

In this Letter, we demonstrate the observation of colorful Airy beams and Airy imaging of letters, which we called Airy letters here, generated through the continuous cubic phase microplate (CCPP) elaborately fabricated by femtosecond laser two-photon processing. The fabricated CCPP with both micro size (60 µm×60 µm×1.1 µm) and continuous variation of phase shows a good agreement with the designed CCPP. Chromatic Airy beams and Airy letters "USTC" are experimentally generated via the CCPP illuminated by white light. In addition, superior properties of Airy letters are explored, demonstrating that the Airy letters inherit the nondiffraction, self-healing, and transverse acceleration characteristics of Airy beams. Our work paves the way toward integrated optics, light separation, optical imaging, and defective information recovery.

Real-time two-photon lithography in controlled flow to create a single-microparticle array and particle-cluster array for optofluidic imaging.

Microarray technology provides an excellent platform for biomedical and biochemical research including basic scientific studies, drug discovery, and diagnostics. Here, we develop a novel method referred to as real-time two-photon lithography in a controlled flow in which femtosecond laser two-photon lithography is performed in situ in the sequential mode stopping and flowing the flow of liquid resin containing microparticles to achieve 100% trapping on a one-bead-to-one-trap basis. Polydisperse particles can be all trapped to form a desired array by freely designing trap structures, resulting in an unprecedentedly high capture efficiency of ∼100%. No persistent pressure is needed after trapping which reduces the complexity of the system. In addition, trapping of particle-cluster arrays with a controlled number of particles is also achieved via this method. The trapped particles inside the microchip are successfully applied as microlenses for high quality imaging. The present technology marks an essential step towards a versatile platform for the integration of bead-based assays and paves the way for developing innovative microfluidics, optofluidics, micro-optics and single-cell analysis devices.

Arch-like microsorters with multi-modal and clogging-improved filtering functions by using femtosecond laser multifocal parallel microfabrication.

Conventional micropore membranes based size sorting have been widely applied for single-cell analysis. However, only a single filtering size can be achieved and the clogging issue cannot be completely avoided. Here, we propose a novel arch-like microsorter capable of multimodal (high-, band- and low-capture mode) sorting of particles. The target particles can pass through the front filter and are then trapped by the back filter, while the non-target particles can bypass or pass through the microsorter. This 3D arch-like microstructures are fabricated inside a microchannel by femtosecond laser parallel multifocal scanning. The designed architecture allows for particles isolation free of clogging over 20 minutes. Finally, as a proof of concept demonstration, SUM159 breast cancer cells are successfully separated from whole blood.

Self-Sealed Bionic Long Microchannels with Thin Walls and Designable Nanoholes Prepared by Line-Contact Capillary-Force Assembly.

Long microchannels with thin walls, small width, and nanoholes or irregular shaped microgaps, which are similar to capillaries or cancerous vessels, are urgently needed to simulate the physiological activities in human body. However, the fabrication of such channels remains challenging. Here, microchannels with designable holes are manufactured by combining laser printing with line-contact capillary-force assembly. Two microwalls are first printed by femtosecond laser direct-writing, and subsequently driven to collapse into a channel by the capillary force that arises in the evaporation of developer. The channel can remain stable in solvent due to the enhanced Van der Waals' force caused by the line-contact of microwalls. Microchannels with controllable nanoholes and almost arbitrary patterns can be fabricated without any bonding or multistep processes. As-prepared microchannels, with wall thicknesses less than 1 µm, widths less than 3 µm, lengths more than 1 mm, are comparable with human capillaries. In addition, the prepared channels also exhibit the ability to steer the flow of liquid without any external pump.

Three-dimensional chiral microstructures fabricated by structured optical vortices in isotropic material.

Optical vortices, a type of structured beam with helical phase wavefronts and 'doughnut'-shaped intensity distributions, have been used to fabricate chiral structures in metals and spiral patterns in anisotropic polarization-dependent azobenzene polymers. However, in isotropic polymers, the fabricated microstructures are typically confined to non-chiral cylindrical geometry due to the two-dimensional 'doughnut'-shaped intensity profile of the optical vortices. Here we develop a powerful strategy to realize chiral microstructures in isotropic material by coaxial interference of a vortex beam and a plane wave, which produces three-dimensional (3D) spiral optical fields. These coaxial interference beams are generated by designing contrivable holograms consisting of an azimuthal phase and an equiphase loaded on a liquid-crystal spatial light modulator. In isotropic polymers, 3D chiral microstructures are achieved under illumination using coaxial interference femtosecond laser beams with their chirality controlled by the topological charge. Our further investigation reveals that the spiral lobes and chirality are caused by interfering patterns and helical phase wavefronts, respectively. This technique is simple, stable and easy to perform, and it offers broad applications in optical tweezers, optical communications and fast metamaterial fabrication.

Optimized holographic femtosecond laser patterning method towards rapid integration of high-quality functional devices in microchannels.

Rapid integration of high-quality functional devices in microchannels is in highly demand for miniature lab-on-a-chip applications. This paper demonstrates the embellishment of existing microfluidic devices with integrated micropatterns via femtosecond laser MRAF-based holographic patterning (MHP) microfabrication, which proves two-photon polymerization (TPP) based on spatial light modulator (SLM) to be a rapid and powerful technology for chip functionalization. Optimized mixed region amplitude freedom (MRAF) algorithm has been used to generate high-quality shaped focus field. Base on the optimized parameters, a single-exposure approach is developed to fabricate 200 × 200 µm microstructure arrays in less than 240 ms. Moreover, microtraps, QR code and letters are integrated into a microdevice by the advanced method for particles capture and device identification. These results indicate that such a holographic laser embellishment of microfluidic devices is simple, flexible and easy to access, which has great potential in lab-on-a-chip applications of biological culture, chemical analyses and optofluidic devices.

High efficiency integration of three-dimensional functional microdevices inside a microfluidic chip by using femtosecond laser multifoci parallel microfabrication.

High efficiency fabrication and integration of three-dimension (3D) functional devices in Lab-on-a-chip systems are crucial for microfluidic applications. Here, a spatial light modulator (SLM)-based multifoci parallel femtosecond laser scanning technology was proposed to integrate microstructures inside a given 'Y' shape microchannel. The key novelty of our approach lies on rapidly integrating 3D microdevices inside a microchip for the first time, which significantly reduces the fabrication time. The high quality integration of various 2D-3D microstructures was ensured by quantitatively optimizing the experimental conditions including prebaking time, laser power and developing time. To verify the designable and versatile capability of this method for integrating functional 3D microdevices in microchannel, a series of microfilters with adjustable pore sizes from 12.2 µm to 6.7 µm were fabricated to demonstrate selective filtering of the polystyrene (PS) particles and cancer cells with different sizes. The filter can be cleaned by reversing the flow and reused for many times. This technology will advance the fabrication technique of 3D integrated microfluidic and optofluidic chips.

Capillary Force Driven Self-Assembly of Anisotropic Hierarchical Structures Prepared by Femtosecond Laser 3D Printing and Their Applications in Crystallizing Microparticles.

The hierarchical structures are the derivation of various functionalities in the natural world and have inspired broad practical applications in chemical systhesis and biological manipulation. However, traditional top-down fabrication approaches suffered from low complexity. We propose a laser printing capillary-assisted self-assembly (LPCS) strategy for fabricating regular periodic structures. Microscale pillars are first produced by the localized femtosecond laser polymerization and are subsequently self-assembled into periodic hierarchical architectures with the assistance of controlled capillary force. Moreover, based on anisotropic assemblies of micropillars, the LPCS method is further developed for the preparation of more complicated and advanced functional microstructures. Pillars cross section, height, and spatial arrangement can be tuned to guide capillary force, and diverse assemblies with different configurations are thus achieved. Finally, we developed a strategy for growing micro/nanoparticles in designed spatial locations through solution-evaporation self-assembly induced by morphology. Due to the high flexibility of LPCS method, the special arrangements, sizes, and distribution density of the micro/nanoparticles can be controlled readily. Our method will be employed not only to fabricate anisotropic hierarchical structures but also to design and manufacture organic/inorganic microparticles.

Laser printing hierarchical structures with the aid of controlled capillary-driven self-assembly.

Capillary force is often regarded as detrimental because it may cause undesired distortion or even destruction to micro/nanostructures during a fabrication process, and thus many efforts have been made to eliminate its negative effects. From a different perspective, capillary force can be artfully used to construct specific complex architectures. Here, we propose a laser printing capillary-assisted self-assembly strategy for fabricating regular periodic structures. Microscale pillars are first produced by localized femtosecond laser polymerization and are subsequently assembled into periodic hierarchical architectures with the assistance of controlled capillary forces in an evaporating liquid. Spatial arrangements, pillar heights, and evaporation processes are readily tuned to achieve designable ordered assemblies with various geometries. Reversibility of the assembly is also revealed by breaking the balance between the intermolecular force and the elastic standing force. We further demonstrate the functionality of the hierarchical structures as a nontrivial tool for the selective trapping and releasing of microparticles, opening up a potential for the development of in situ transportation systems for microobjects.