Biotinylated Photopolymers for 3D‐Printed Unibody Lab‐on‐a‐Chip Optical Platforms

The present work reports the first demonstration of straightforward fabrication of monolithic unibody lab‐on‐a‐chip (ULOCs) integrating bioactive micrometric 3D scaffolds by means of multimaterial stereolithography (SL). To this end, a novel biotin‐conjugated photopolymer is successfully synthesized and optimally formulated to achieve high‐performance SL‐printing resolution, as demonstrated by the SL‐fabrication of biotinylated structures smaller than 100 µm. By optimizing a multimaterial single‐run SL‐based 3D‐printing process, such biotinylated microstructures are incorporated within perfusion microchambers whose excellent optical transparency enables real‐time optical microscopy analyses. Standard biotin‐binding assays confirm the existence of biotin‐heads on the surfaces of the embedded 3D microstructures and allow to demonstrate that the biofunctionality of biotin is not altered during the SL‐printing, thus making it exploitable for further conjugation with other biomolecules. As a step forward, an in‐line optical detection system is designed, prototyped via SL‐printing and serially connected to the perfusion microchambers through customized world‐to‐chip connectors. Such detection system is successfully employed to optically analyze the solution flowing out of the microchambers, thus enabling indirect quantification of the concentration of target interacting biomolecules. The successful application of this novel biofunctional photopolymer as SL‐material enables to greatly extend the versatility of SL to directly fabricate ULOCs with intrinsic biofunctionality.     

A Solution‐Processable,Omnidirectionally Stretchable,and High‐Pressure‐Sensitive Piezoresistive Device

The development of omnidirectionally stretchable pressure sensors with high performance without stretching‐induced interference has been hampered by many challenges. Herein, an omnidirectionally stretchable piezoresistive pressure‐sensing device is demonstrated by combining an omniaxially stretchable substrate with a 3D micropattern array and solution‐printing of electrode and piezoresistive materials. A unique substrate structural design and materials mean that devices that are highly sensitive are rendered, with a stable out‐of‐plane pressure response to both static (sensitivity of 0.5 kPa^?1 and limit of detection of 28 Pa) and dynamic pressures and the minimized in‐plane stretching responsiveness (a small strain gauge factor of 0.17), achieved through efficient strain absorption of the electrode and sensing materials. The device can detect human‐body tremors, as well as measure the relative elastic properties of human skin. The omnidirectionally stretchable pressure sensor with a high pressure sensitivity and minimal stretch‐responsiveness yields great potential to skin‐attachable wearable electronics, human–machine interfaces, and soft robotics applications.     

High‐Density Microfluidic Particle‐Cluster‐Array Device for Parallel and Dynamic Study of Interaction between Engineered Particles

A high‐density and high‐performance microfluidic particle‐cluster‐array device utilizing a novel hydrodynamically tunable pneumatic valve (HTPV) is reported for parallel and dynamic monitoring of the interactions taking place in particle clusters. The key concept involves passive operation of the HTPV through elastic deformation of a thin membrane using only the hydrodynamic force inherent in microchannel flows. This unique feature allows the discrete and high‐density (≈30 HTPVs mm^?2) arrangement of numerous HTPVs in a microfluidic channel without any pneumatic connection. In addition, the HTPV achieves high‐performance clustering (≈92%) of three different particles in an array format through the optimization of key design and operating parameters. Finally, a contamination‐free, parallel, and dynamic biochemical analysis strategy is proposed, which employs a simple one‐inlet–one‐outlet device operated by the effective combination of several techniques, including particle clustering, the interactions between engineered particles, two‐phase partitioning and dehydration control of aqueous plugs, and shape/color‐based particle identification.     

Design of a Microchannel‐Nanochannel‐Microchannel Array Based Nanoelectroporation System for Precise Gene Transfection

A micro/nano‐fabrication process of a nanochannel electroporation (NEP) array and its application for precise delivery of plasmid for non‐viral gene transfection is described. A dip‐combing device is optimized to produce DNA nanowires across a microridge array patterned on the polydimethylsiloxane (PDMS) surface with a yield up to 95%. Molecular imprinting based on a low viscosity resin, 1,4‐butanediol diacrylate (1,4‐BDDA), adopted to convert the microridge‐nanowire‐microridge array into a microchannel‐nanochannel‐microchannel (MNM) array. Secondary machining by femtosecond laser ablation is applied to shorten one side of microchannels from 3000 to 50 μm to facilitate cell loading and unloading. The biochip is then sealed in a packaging case with reservoirs and microfluidic channels to enable cell and plasmid loading, and to protect the biochip from leakage and contamination. The package case can be opened for cell unloading after NEP to allow for the follow‐up cell culture and analysis. These NEP cases can be placed in a spinning disc and up to ten discs can be piled together for spinning. The resulting centrifugal force can simultaneously manipulate hundreds or thousands of cells into microchannels of NEP arrays within 3 minutes. To demonstrate its application, a 13 kbp OSKM plasmid of induced pluripotent stem cell (iPSC) is injected into mouse embryonic fibroblasts cells (MEFCs). Fluorescence detection of transfected cells within the NEP biochips shows that the delivered dosage is high and much more uniform compared with similar gene transfection carried out by the conventional bulk electroporation (BEP) method.     

A two‐dimensional stochastic algorithm for the solution of the non‐linear Poisson–Boltzmann equation: validation with finite‐difference benchmarks

This paper presents a two‐dimensional floating random walk (FRW) algorithm for the solution of the non‐linear Poisson–Boltzmann (NPB) equation. In the past, the FRW method has not been applied to the solution of the NPB equation which can be attributed to the absence of analytical expressions for volumetric Green's functions. Previous studies using the FRW method have examined only the linearized Poisson–Boltzmann equation. No such linearization is needed for the present approach. Approximate volumetric Green's functions have been derived with the help of perturbation theory, and these expressions have been incorporated within the FRW framework. A unique advantage of this algorithm is that it requires no discretization of either the volume or the surface of the problem domains. Furthermore, each random walk is independent, so that the computational procedure is highly parallelizable. In our previous work, we have presented preliminary calculations for one‐dimensional and quasi‐one‐dimensional benchmark problems. In this paper, we present the detailed formulation of a two‐dimensional algorithm, along with extensive finite‐difference validation on fully two‐dimensional benchmark problems. The solution of the NPB equation has many interesting applications, including the modelling of plasma discharges, semiconductor device modelling and the modelling of biomolecular structures and dynamics. Copyright © 2005 John Wiley & Sons, Ltd.     

Aligning Solution‐Derived Carbon Nanotube Film with Full Surface Coverage for High‐Performance Electronics Applications

The main challenge for application of solution‐derived carbon nanotubes (CNTs) in high performance field‐effect transistor (FET) is how to align CNTs into an array with high density and full surface coverage. A directional shrinking transfer method is developed to realize high density aligned array based on randomly orientated CNT network film. Through transferring a solution‐derived CNT network film onto a stretched retractable film followed by a shrinking process, alignment degree and density of CNT film increase with the shrinking multiple. The quadruply shrunk CNT films present well alignment, which is identified by the polarized Raman spectroscopy and electrical transport measurements. Based on the high quality and high density aligned CNT array, the fabricated FETs with channel length of 300 nm present ultrahigh performance including on‐state current I_on of 290 µA µm^?1 (V_ds = ?1.5 V and V_gs = ?2 V) and peak transconductance g_m of 150 µS µm^?1, which are, respectively, among the highest corresponding values in the reported CNT array FETs. High quality and high semiconducting purity CNT arrays with high density and full coverage obtained through this method promote the development of high performance CNT‐based electronics.     

Direct Synthesis of a Self‐Assembled WSe2/MoS2 Heterostructure Array and its Optoelectrical Properties

Functional van der Waals heterojunctions of transition metal dichalcogenides are emerging as a potential candidate for the basis of next‐generation logic devices and optoelectronics. However, the complexity of synthesis processes so far has delayed the successful integration of the heterostructure device array within a large scale, which is necessary for practical applications. Here, a direct synthesis method is introduced to fabricate an array of self‐assembled WSe₂/MoS₂ heterostructures through facile solution‐based directional precipitation. By manipulating the internal convection flow (i.e., Marangoni flow) of the solution, the WSe₂ wires are selectively stacked over the MoS₂ wires at a specific angle, which enables the formation of parallel‐ and cross‐aligned heterostructures. The realized WSe₂/MoS₂‐based p–n heterojunction shows not only high rectification (ideality factor: 1.18) but also promising optoelectrical properties with a high responsivity of 5.39 A W^?1 and response speed of 16 µs. As a feasible application, a WSe₂/MoS₂‐based photodiode array (10 × 10) is demonstrated, which proves that the photosensing system can detect the position and intensity of an external light source. The solution‐based growth of hierarchical structures with various alignments could offer a method for the further development of large‐area electronic and optoelectronic applications.     

Fabrication of Flexible MoS2 Thin‐Film Transistor Arrays for Practical Gas‐Sensing Applications

By combining two kinds of solution‐processable two‐dimensional materials, a flexible transistor array is fabricated in which MoS₂ thin film is used as the active channel and reduced graphene oxide (rGO) film is used as the drain and source electrodes. The simple device configuration and the 1.5 mm‐long MoS₂ channel ensure highly reproducible device fabrication and operation. This flexible transistor array can be used as a highly sensitive gas sensor with excellent reproducibility. Compared to using rGO thin film as the active channel, this new gas sensor exhibits much higher sensitivity. Moreover, functionalization of the MoS₂ thin film with Pt nanoparticles further increases the sensitivity by up to ～3 times. The successful incorporation of a MoS₂ thin‐film into the electronic sensor promises its potential application in various electronic devices.     

Fabrication of microchambers defined by photopolymerized hydrogels and weirs within microfluidic systems: application to DNA hybridization

This paper describes fabrication of serial microchamber arrays within the channels of a microfluidic device. The chambers are defined using a combination of weirs and UV-cross-linked hydrogel plugs (poly(ethylene glycol) diacrylates). This approach permits the microchambers to be addressed by pump-driven pressure in one dimension and by electrophoresis in the other. The function of the device is demonstrated by detecting DNA targets. Single-strand DNA (ssDNA) probes labeled with biotin were immobilized onto microbeads coated with streptavidin. The DNA-functionalized microbeads were packed into each of three microchambers by injection through inlet wells. Three oligonucleotides were designed as probes and four as targets. Hybridization reactions were performed by moving the targets across the array of probe-containing microchambers by electrophoresis. The hybridization of fluorescein-labeled ssDNA targets to complementary probes was observed by fluorescence microscopy. These studies resulted in four key observations: (1) there was no detectable binding of targets to noncomplementary probes; (2) hybridization was 90% complete within 1 min; (3) once captured, the targets could be independently released and recovered from the microbeads by treatment with 0.1 N NaOH; (4) multiple analyses could be performed using a single bead set, but there was degradation in performance after each capture/release cycle.     

A Self‐Organized Poly(vinylpyrrolidone)‐Based Cathode Interlayer in Inverted Fullerene‐Free Organic Solar Cells

Herein, poly(vinylpyrrolidone) (PVP) is used as the cathode interlayer (CIL) through the self‐organization method in inverted organic solar cells (OSCs). By coating a solution of PVP and active layer materials onto a glass/indium tin oxide (ITO) substrate, the PVP can segregate to the near ITO side due to its high surface energy and strong intermolecular interaction with the ITO electrode. The power conversion efficiency (PCE) of the obtained OSC device reaches 13.3%, much higher than that of the control device with a PCE of only 10.1%. The improvement results from the increased exciton dissociation efficiency and the depressed trap‐assisted recombination, which can be attributed to the reduced work function of the cathode by the self‐organized PVP. Additionally, the molecular weight of the PVP has almost no influence on the device performance, and the PVP‐modified device presents superior stability. This method can also be applied in other highly efficient fullerene‐free OSCs, and with a fine selection of the active layer, a high PCE of 14.0% is obtained. Overall, this work demonstrates the great potential of the PVP‐based CIL in inverted OSCs fabricated via the self‐organization method.     

Environmentally Friendly Solvent‐Processed Organic Solar Cells that are Highly Efficient and Adaptable for the Blade‐Coating Method

The power conversion efficiencies (PCEs) of state‐of‐the‐art organic solar cells (OSCs) have increased to over 13%. However, the most commonly used solvents for making the solutions of photoactive materials and the coating methods used in laboratories are not adaptable for future practical production. Therefore, taking a solution‐coating method with environmentally friendly processing solvents into consideration is critical for the practical utilization of OSC technology. In this study, a highly efficient PBTA‐TF:IT‐M‐based device processed with environmentally friendly solvents, tetrahydrofuran/isopropyl alcohol (THF/IPA) and o‐xylene/1‐phenylnaphthalene, is fabricated; a high PCE of 13.1% can be achieved by adopting the spin‐coating method, which is the top result for OSCs. More importantly, a blade‐coated non‐fullerene OSC processed with THF/IPA is demonstrated for the first time to obtain a promising PCE of 11.7%; even for the THF/IPA‐processed large‐area device (1.0 cm²) made by blade‐coating, a PCE of 10.6% can still be maintained. These results are critical for the large‐scale production of highly efficient OSCs in future studies.     

Templated Self‐Assembly of Block Copolymers: Top‐Down Helps Bottom‐Up

One of the key challenges in nanotechnology is to control a self‐assembling system to create a specific structure. Self‐organizing block copolymers offer a rich variety of periodic nanoscale patterns, and researchers have succeeded in finding conditions that lead to very long range order of the domains. However, the array of microdomains typically still contains some uncontrolled defects and lacks global registration and orientation. Recent efforts in templated self‐assembly of block copolymers have demonstrated a promising route to control bottom‐up self‐organization processes through top‐down lithographic templates. The orientation and placement of block‐copolymer domains can be directed by topographically or chemically patterned templates. This templated self‐assembly method provides a path towards the rational design of hierarchical device structures with periodic features that cover several length scales.     

High‐Performance Solution‐Processed Organo‐Metal Halide Perovskite Unipolar Resistive Memory Devices in a Cross‐Bar Array Structure

Resistive random access memories can potentially open a niche area in memory technology applications by combining the advantages of the long endurance of dynamic random‐access memory and the long retention time of flash memories. Recently, resistive memory devices based on organo‐metal halide perovskite materials have demonstrated outstanding memory properties, such as a low‐voltage operation and a high ON/OFF ratio; such properties are essential requirements for low power consumption in developing practical memory devices. In this study, a nonhalide lead source is employed to deposit perovskite films via a simple single‐step spin‐coating method for fabricating unipolar resistive memory devices in a cross‐bar array architecture. These unipolar perovskite memory devices achieve a high ON/OFF ratio up to 10⁸ with a relatively low operation voltage, a large endurance, and long retention times. The high‐yield device fabrication based on the solution‐process demonstrated here will be a step toward achieving low‐cost and high‐density practical perovskite memory devices.     

Constrained total least‐squares computations for high‐resolution image reconstruction with multisensors

Multiple undersampled images of a scene are often obtained by using a charge‐coupled device (CCD) detector array of sensors that are shifted relative to each other by subpixel displacements. This geometry of sensors, where each sensor has a subarray of sensing elements of suitable size, has been popular in the task of attaining spatial resolution enhancement from the acquired low‐resolution degraded images that comprise the set of observations. With the objective of improving the performance of the signal processing algorithms in the presence of the ubiquitous perturbation errors of displacements around the ideal subpixel locations (because of imperfections in fabrication), in addition to noisy observation, the errors‐in‐variables or the total least‐squares method is used in this paper. A regularized constrained total least‐squares (RCTLS) solution to the problem is given, which requires the minimization of a nonconvex and nonlinear cost functional. Simulations indicate that the choice of the regularization parameter influences significantly the quality of the solution. The L‐curve method is used to select the theoretically optimum value of the regularization parameter instead of the unsound but expedient trial‐and‐error approach. The expected superiority of this RCTLS approach over the conventional least‐squares theory‐based algorithm is substantiated by example. © 2002 John Wiley & Sons, Inc. Int J Imaging Syst Technol 12, 35–42, 2002     

Boundary elements for half‐space problems via fundamental solutions: A three‐dimensional analysis

An efficient solution technique is proposed for the three‐dimensional boundary element modelling of half‐space problems. The proposed technique uses alternative fundamental solutions of the half‐space (Mindlin's solutions for isotropic case) and full‐space (Kelvin's solutions) problems. Three‐dimensional infinite boundary elements are frequently employed when the stresses at the internal points are required to be evaluated. In contrast to the published works, the strongly singular line integrals are avoided in the proposed solution technique, while the discretization of infinite elements is independent of the finite boundary elements. This algorithm also leads to a better numerical accuracy while the computational time is reduced. Illustrative numerical examples for typical isotropic and transversely isotropichalf‐space problems demonstrate the potential applications of the proposed formulations. Incidentally, the results of the illustrative examples also provide a parametric study for the imperfect contact problem. Copyright © 2001 John Wiley & Sons, Ltd.     

Advanced SERS Sensor Based on Capillarity‐Assisted Preconcentration through Gold Nanoparticle‐Decorated Porous Nanorods

A preconcentrating surface‐enhanced Raman scattering (SERS) sensor for the analysis of liquid‐soaked tissue, tiny liquid droplets and thin liquid films without the necessity to collect the analyte is reported. The SERS sensor is based on a block‐copolymer membrane containing a spongy‐continuous pore system. The sensor's upper side is an array of porous nanorods having tips functionalized with Au nanoparticles. Capillarity in combination with directional evaporation drives the analyte solution in contact with the flat yet nanoporous underside of the SERS sensor through the continuous nanopore system toward the nanorod tips where non‐volatile components of the analyte solution precipitate at the Au nanoparticles. The nanorod architecture increases the sensor surface in the detection volume and facilitates analyte preconcentration driven by directional solvent evaporation. The model analyte 5,5′‐dithiobis(2‐nitrobenzoic acid) can be detected in a 1 × 10^?3m solution ≈300 ms after the sensor is brought into contact with the solution. Moreover, a sensitivity of 0.1 ppm for the detection of the dissolved model analyte is achieved.     

On-chip nanoliter-volume multiplex TaqMan polymerase chain reaction from a single copy based on counting fluorescence released microchambers

A novel method for multiplex TaqMan PCR in nanoliter volumes on a highly integrated silicon microchamber array is described. Three different gene targets, related to beta-actin, sex-determining region Y (SRY), and Rhesus D (RhD) were amplified and detected simultaneously on the same chip by using three different types of human genomic DNA as the templates. The lack of cross-contamination and carryover was shown using alternate dispensing of mineral oil-coated microchambers containing template and those without template. To confirm the specificity of our system to beta-actin, SRY, and RhD genes, we employed the larger volume PCR samples to a commercial real-time PCR system, SmartCycler. The samples were cycled with the same sustaining temperatures as with the microchamber array. Instead of the conventional method of DNA quantification, counting the number of the fluorescence released microchambers in consequence to TaqMan PCR was employed to our chip. This simple method of observing the end point signal had provided a dynamic quantitative range. Stochastic amplification of 0.4 copies/reaction chamber was achieved. The microfabricated PCR chip demonstrated a rapid and highly sensitive response for simultaneous multiple-target detection, which is a promising step toward the development of a fully integrated device for the "lab-on-a-chip" DNA analysis.     

A Novel Phase‐Transformation Activation Process toward Ni–Mn–O Nanoprism Arrays for 2.4 V Ultrahigh‐Voltage Aqueous Supercapacitors

One of the key challenges of aqueous supercapacitors is the relatively low voltage (0.8–2.0 V), which significantly limits the energy density and feasibility of practical applications of the device. Herein, this study reports a novel Ni–Mn–O solid‐solution cathode to widen the supercapacitor device voltage, which can potentially suppress the oxygen evolution reaction and thus be operated stably within a quite wide potential window of 0–1.4 V (vs saturated calomel electrode) after a simple but unique phase‐transformation electrochemical activation. The solid‐solution structure is designed with an ordered array architecture and in situ nanocarbon modification to promote the charge/mass transfer kinetics. By paring with commercial activated carbon anode, an ultrahigh voltage asymmetric supercapacitor in neutral aqueous LiCl electrolyte is assembled (2.4 V; among the highest for single‐cell supercapacitors). Moreover, by using a polyvinyl alcohol (PVA)–LiCl electrolyte, a 2.4 V hydrogel supercapacitor is further developed with an excellent Coulombic efficiency, good rate capability, and remarkable cycle life (>5000 cycles; 95.5% capacity retention). Only one cell can power the light‐emitting diode indicator brightly. The resulting maximum volumetric energy density is 4.72 mWh cm^?3, which is much superior to previous thin‐film manganese‐oxide‐based supercapacitors and even battery–supercapacitor hybrid devices.     

Solution‐Processed Wide‐Bandgap Organic Semiconductor Nanostructures Arrays for Nonvolatile Organic Field‐Effect Transistor Memory

In this paper, the development of organic field‐effect transistor (OFET) memory device based on isolated and ordered nanostructures (NSs) arrays of wide‐bandgap (WBG) small‐molecule organic semiconductor material [2‐(9‐(4‐(octyloxy)phenyl)‐9H‐fluoren‐2‐yl)thiophene]3 (WG₃) is reported. The WG₃ NSs are prepared from phase separation by spin‐coating blend solutions of WG₃/trimethylolpropane (TMP), and then introduced as charge storage elements for nonvolatile OFET memory devices. Compared to the OFET memory device with smooth WG₃ film, the device based on WG₃ NSs arrays exhibits significant improvements in memory performance including larger memory window (≈45 V), faster switching speed (≈1 s), stable retention capability (>10⁴ s), and reliable switching properties. A quantitative study of the WG₃ NSs morphology reveals that enhanced memory performance is attributed to the improved charge trapping/charge‐exciton annihilation efficiency induced by increased contact area between the WG₃ NSs and pentacene layer. This versatile solution‐processing approach to preparing WG₃ NSs arrays as charge trapping sites allows for fabrication of high‐performance nonvolatile OFET memory devices, which could be applicable to a wide range of WBG organic semiconductor materials.     

Simultaneous Measurements of Geometric and Viscoelastic Properties of Hydrogel Microbeads Using Continuous‐Flow Microfluidics with Embedded Electrodes

Geometric and mechanical characterizations of hydrogel materials at the microscale are attracting increasing attention due to their importance in tissue engineering, regenerative medicine, and drug delivery applications. Contemporary approaches for measuring the these properties of hydrogel microbeads suffer from low‐throughput, complex system configuration, and measurement inaccuracy. In this work, a continuous‐flow device is developed to measure geometric and viscoelastic properties of hydrogel microbeads by flowing the microbeads through a tapered microchannel with an array of interdigitated microelectrodes patterned underneath the channel. The viscoelastic properties are derived from the trajectories of microbeads using a quasi‐linear viscoelastic model. The measurement is independent of the applied volumetric flow rate. The results show that the geometric and viscoelastic properties of Ca‐alginate hydrogel microbeads can be determined independently and simultaneously. The bulky high‐speed optical systems are eliminated, simplifying the system configuration and making it a truly miniaturized device. A throughput of up to 394 microbeads min^?1 is achieved. This study may provide a powerful tool for mechanical profiling of hydrogel microbeads to support their wide applications.