Smart Droplet Microfluidic System for Single-Cell Selective Lysis and Real-Time Sorting Based on Microinjection and Image Recognition.

Single-cell analysis has important implications for understanding the specificity of cells. To analyze the specificity of rare cells in complex blood and biopsy samples, selective lysis of target single cells is pivotal but difficult. Microfluidics, particularly droplet microfluidics, has emerged as a promising tool for single-cell analysis. In this paper, we present a smart droplet microfluidic system that allows for single-cell selective lysis and real-time sorting, aided by the techniques of microinjection and image recognition. A custom program evolved from Python is proposed for recognizing target droplets and single cells, which also coordinates the operation of various parts in a whole microfluidic system. We have systematically investigated the effects of voltage and injection pressure applied to the oil-water interface on droplet microinjection. An efficient and selective droplet injection scheme with image feedback has been demonstrated, with an efficiency increased dramatically from 2.5% to about 100%. Furthermore, we have proven that the cell lysis solution can be selectively injected into target single-cell droplets. Then these droplets are shifted into the sorting area, with an efficiency for single K562 cells reaching up to 73%. The system function is finally explored by introducing complex cell samples, namely, K562 cells and HUVECs, with a success rate of 75.2% in treating K562 cells as targets. This system enables automated single-cell selective lysis without the need for manual handling and sheds new light on the cooperation with other detection techniques for a broad range of single-cell analysis.

Microwell Confined Electro-Coalescence for Rapid Formation of High-Throughput Droplet Array.

Droplet array is widely applied in single cell analysis, drug screening, protein crystallization, etc. This work proposes and validates a method for rapid formation of uniform droplet array based on microwell confined droplets electro-coalescence of screen-printed emulsion droplets, namely electro-coalescence droplet array (ECDA). The electro-coalescence of droplets is according to the polarization induced electrostatic and dielectrophoretic forces, and the dielectrowetting effect. The photolithographically fabricated microwells are highly regular and reproducible, ensuring identical volume and physical confinement to achieve uniform droplet array, and meanwhile the microwell isolation protects the paired water droplets from further fusion and broadens its feasibility to different fluidic systems. Under optimized conditions, a droplet array with an average diameter of 85 µm and a throughput of 106 in a 10 cm × 10 cm chip can be achieved within 5 s at 120 Vpp and 50 kHz. This ECDA chip is validated for various microwell geometries and functional materials. The optimized ECDA are successfully applied for digital viable bacteria counting, showing comparable results to the plate culture counting. Such an ECDA chip, as a digitizable and high-throughput platform, presents excellent potential for high-throughput screening, analysis, absolute quantification, etc.

Generation and control of the circle Olver beams.

The circle Olver beams (COBs) generated by modulation on the basis of a new type of Olver beam are presented numerically and experimentally. The zeroth order COB is the circle Airy beam. We demonstrate auto-focusing of the COBs with both inward and outward accelerations, where the odd order COBs display auto-defocusing while the even order COBs (ECOBs) tend to focus more abruptly. We also explore the effect of the decay factor and the scaling factor on the beams' focusing properties, such as the initial energy distribution, the focusing position, the focusing intensity and the focusing depth, by using the parity mode. In addition, we verify the self-healing property of the COBs. Finally, we set up an experimental platform to implement particle capture and manipulation with the ECOBs. Our results offer practical applications for particle manipulation, laser processing, etc.

Generation and control of the circle Olver beams: erratum.

We have found an error in our work reported in [Opt. Express31(4), 6241 (2023)10.1364/OE.483433], which we correct in this erratum. The authors apologize for this error and emphasize that none of the results are affected by this error.

Replaceable Dielectric Film for Low-Voltage and High-Performance Electrowetting-Based Digital Microfluidics.

Electrowetting-on-dielectric (EWOD) technology has been considered as a promising candidate for digital microfluidic (DMF) applications due to its outstanding flexibility and integrability. The dielectric layer with a hydrophobic surface is the key element of an EWOD device, determining its driving voltage, reliability, and lifetime. Hereby, inspired by the ionic-liquid-filled structuring polymer with high capacitance independent on thickness, namely ion gel (IG), we develop a polymer (P)-ion gel-amorphous fluoropolymer, namely, PIGAF, composite film as a replaceable hydrophobic dielectric layer for fabrication of a high-efficiency and stable EWOD-DMF device at relatively low voltage. The results show that the proposed EWOD devices using the PIGAF-based dielectric layer can achieve a large contact angle (θ) change of ∼50° and excellent reversibility with a contact angle hysteresis of ≤5° at a relatively low voltage of 30 Vrms. More importantly, the EWOD actuation voltage did not change obviously with the PIGAF film thickness in the range of several to tens of microns, enabling the thickness of the film to be adjusted according to the demand within a certain range while keeping the actuation voltage low. An EWOD-DMF device can be prepared by simply stacking a PIGAF film onto a PCB board, demonstrating stable droplet actuation (motion) at 30 Vrms and 1 kHz as well as a maximum moving velocity of 69 mm/s at 140 Vrms and 1 kHz. The PIGAF film was highly stable and reliable, maintaining excellent EWOD performance after multiple droplet manipulations (≥50 cycles) or long-term storage of 1 year. The proposed EWOD-DMF device has been demonstrated for digital chemical reactions and biomedical sensing applications.

High quality stealth dicing of sapphire with a picosecond Bessel beam by controlling the polarization direction.

Sapphire is an important substrate material in optoelectronic devices, and it is also widely used as a touch screen panel. In order to achieve high quality cutting of sapphire, the stealth dicing of 500 µm thick sapphire by a picosecond Bessel beam is studied in this paper. The influences of laser polarization direction and process parameters on cutting section roughness were studied. By controlling the laser polarization direction, different crack propagation morphologies were obtained. When the polarization direction was vertical to the cutting path, the crack propagation path was straighter, and the sapphire had better cutting quality. The laser processing parameters, including burst mode, hole spacing, and pulse energy, had a significant impact on the cutting section roughness. When the polarization direction was vertical to the cutting path under the optimal process parameters, the cutting section was uniform and flat, with no recondensable particles, no ripples, and no chamfer, and an 89.7 nm average roughness of the cutting section could be obtained.

Porous organic polymers for Li-chemistry-based batteries: functionalities and characterization studies.

Porous organic polymers (POPs), a versatile class of materials that possess many tunable properties such as high chemical absorptivity and ionic conductivity, are emerging candidate electrode materials, permselective membranes, ionic conductors, interfacial stabilizers and functional precursors to synthesize advanced porous carbon. Based on their crystal structure features, the emerging POPs can be classified into two subclasses: amorphous POPs (hyper cross-linked polymers, polymers with intrinsic microporosity, conjugated microporous polymers, porous aromatic frameworks, etc.) and crystalline POPs (covalent organic frameworks, etc.). This tutorial review provides a brief introduction of different types of POPs in terms of their classification and functions for tackling the remaining challenges in various types of Li-chemistry-based batteries. In situ and ex situ characterization studies are also discussed to highlight their importance and applicability for the structural investigation of POPs to reveal the underlying mechanism of POPs over the course of the electrochemical process. Although some revolutionary advances have been achieved, the development of POPs in Li-chemistry-based batteries is still in its infancy. Perspectives regarding future application and mechanistic insights of POPs in battery studies are outlined at the end.

Accelerated Multi-step Sulfur Redox Reactions in Lithium-Sulfur Batteries Enabled by Dual Defects in Metal-Organic Framework-based Catalysts.

The sluggish sulfur redox kinetics and shuttle effect of lithium polysulfides (LiPSs) are recognized as the main obstacles to the practical applications of the lithium-sulfur (Li-S) batteries. Accelerated conversion by catalysis can mitigate these issues, leading to enhanced Li-S performance. However, a catalyst with single active site cannot simultaneously accelerate multiple LiPSs conversion. Herein, we developed a novel dual-defect (missing linker and missing cluster defects) metal-organic framework (MOF) as a new type of catalyst to achieve synergistic catalysis for the multi-step conversion reaction of LiPSs. Electrochemical tests and first-principle density functional theory (DFT) calculations revealed that different defects can realize targeted acceleration of stepwise reaction kinetics for LiPSs. Specifically, the missing linker defects can selectively accelerate the conversion of S8 →Li2 S4 , while the missing cluster defects can catalyze the reaction of Li2 S4 →Li2 S, so as to effectively inhibit the shuttle effect. Hence, the Li-S battery with an electrolyte to sulfur (E/S) ratio of 8.9 mL g-1 delivers a capacity of 1087 mAh g-1 at 0.2 C after 100 cycles. Even at high sulfur loading of 12.9 mg cm-2 and E/S=3.9 mL g-1 , an areal capacity of 10.4 mAh cm-2 for 45 cycles can still be obtained.

Polarization and incidence insensitive analogue of electromagnetically induced reflection metamaterial with high group delay.

In this work, we demonstrate an analogue of electromagnetically induced reflection (EIR) effect with hybrid structure consisting of a silica (SiO2) square array layer embedded in graphene-dielectric-Au film constructed F-P cavity. It is shown that the SiO2 square array and F-P cavity create transverse waveguide with high quality factor (Q-factor) and longitudinal F-P modes, and their destructive interference effectively forms the EIR-like effect, which benefits for obtaining high group delay. In addition, the C4 symmetric structure ensures the polarization-independent for this EIR-like effect. With high Q-factor at the reflection window, the ultra-high group delay as high as 245 ps can be obtained. This structure will be useful to develop the EIT-like devices with excellent performance such as high group delay, polarization and incident insensitivity, and environmental stability.

Generation and control of tornado waves by means of ring swallowtail vortex beams.

Tornado waves (ToWs), which refer to a light that accelerates and twists over both the radial and the angular directions, have gained a great deal of interest since the concept was introduced by Brimis et al [Opt. Lett.45, 280 (2020)10.1364/OL.45.000280]. In this paper, we superimpose two pairs of ring swallowtail vortex beams (RSVBs) to generate ToWs and we call them tornado swallowtail waves (ToSWs). Each pair consists of RSVBs while carrying orbital angular momentum of opposite helicity and slightly different with the radius of the main ring of RSVBs. The waves spiral forward and reveal intensity maxima, exhibiting a tornado-like intensity profile during propagation. Meanwhile, the angular acceleration of the ToSWs is illustrated via tracing the angular position of the high-intensity main lobes. It is found that ToSWs present very high values of angular acceleration. Compared with typical tornado waves, ToSWs are more diverse and tunable, giving a new degree of freedom to tailor the propagation dynamics due to the flexibility of the swallowtail diffraction catastrophe. In addition, we confirm such waves experimentally and the results match well with the numerical ones. Also, we demonstrate the ability of optical manipulation of ToSWs for the first time in that they allow for particles not only to be trapped but also to be rotated. Finally, we analyze the poynting vectors and power exchange of ToSWs to demonstrate convincingly the physical mechanism.

Autofocusing self-imaging: symmetric Pearcey Talbot-like effect.

The Talbot-like effect of symmetric Pearcey beams (SPBs) is presented numerically and experimentally in the free space. Owing to the Talbot-like effect, the SPBs have the property of periodic, multiple autofocusing and self-healing. Meanwhile, the focusing positions and focusing times of SPBs are controlled by the beam shift factor and the distribution factors. Furthermore, the beam shift factor can also affect the Talbot-like effect and the Talbot period. It is believed that the results can diversify the application of the Talbot effect.

Multiple and off-axis optical bottles from the chirped circular Pearcey Gaussian vortex beams.

We introduce a new type of multiple and off-axis optical bottles (OBs) based on the chirped circular Pearcey Gaussian vortex beam. This kind of beam allows the generation of the OBs with a perfect bottle shape through coherent superposition. Also, we show that the number and the position of the OBs can be precisely and flexibly controlled. The experimental results agree well with our numerical simulations, and we observe stable trapping of the mesocarbon microbeads particles by the proposed bottle beam.

Shaping autofocusing Airy beams through the modification of Fourier spectrum.

A new type of Airy beam arisen from the modification of Fourier spectrum is introduced numerically and experimentally. The autofocusing Airy beam (AAB) exhibits the features of off-axis autofocusing and transverse self-accelerating, producing a needle-like focus in the longitudinal direction and a tiny focal spot at the focusing plane. Furthermore, the focusing properties such as focusing position, focal spot size, focusing intensity and depth of focus can be adjusted by modulating parameters of the AAB. Experimental demonstrations of particle trapping and manipulation with the AAB are also presented. The number of trapped particles can be controlled by changing the focal spot size at the autofocusing plane. Our results offer practical applications in particle manipulation, fluorescent imaging technology, laser spectroscopy and so on.

Asymmetrical inseparable coherent structures.

A novel, to the best of our knowledge, class of coherent structures of inseparability, incorporating phases asymmetrically cross-coupled by two position vectors, is introduced in theory and experiment. These phases disappear in the environment of complete coherence, but the vanishment is avoidable in the coexistent state of extreme incoherence and full coherence. The radiated beams intrinsically possess a controllable rotation but undergo an intermediate process quite different from the twisted Gaussian Schell-model beams. Analysis shows a novel association between the magnitude and the phase of the coherent structure which displays both synergy and opposition. Our work further reveals the inner mechanism of the inseparable coherent structures and extends a new horizon for the optical twist.

Microfluidic Magnetic Analyte Delivery Technique for Separation, Enrichment, and Fluorescence Detection of Ultratrace Biomarkers.

A microfluidic magnetic analyte delivery (µMAD) technique was developed to realize sample preparation and ultrasensitive biomarker detection. A simply designed microfluidic device was employed to carry out this technique, including a poly(dimethylsiloxane)-glass hybrid microchip having four straight rectangular channels and a permanent magnet. In the µMAD process, functionalized magnetic beads (MBs) were used to recognize and isolate analytes from a complex sample matrix, deliver analytes into tiny microchannels, and preconcentrate analytes in the magnetic trapping/detection region for in situ fluorescence detection. In the feasibility study and sensitivity optimization, horseradish peroxidase-labeled MBs were used, and critical parameters for the signal amplification performance of µMAD were carefully evaluated. At optimized conditions, a sensitivity improvement of at least 2 orders of magnitude was achieved. As a proof of concept, µMAD was combined with the enzyme-linked immunosorbent assay (ELISA), while carcinoembryonic antigen (CEA), prostate-specific antigen (PSA), and interleukin 6 (IL-6) were selected as model biomarkers. The limits of detection (LODs) of µMAD-ELISA were as low as 0.29 pg/mL for CEA, 0.047 pg/mL for PSA, and 0.021 pg/mL for IL-6, which corresponded to an over 200-fold reduction compared to their commercial ELISA results. Meanwhile, µMAD-ELISA revealed high selectivity and reproducibility. In clinical sample analysis, good accuracy was acquired for human serum analysis relative to commercial ELISA kits, and satisfied recoveries of 85.1-102% with RSDs of 1.7-9.8% for IL-6 and 84.7-113% with RSDs of 3.2-8.3% for interferon-γ were obtained. This ultrasensitive and easy operation technique provides a valuable approach for trace-level biomarker detection for practical applications.

Flow-Field-Assisted Dielectrophoretic Microchips for High-Efficiency Sheathless Particle/Cell Separation with Dual Mode.

Prefocusing of cell mixtures through sheath flow is a common technique used for continuous and high-efficiency dielectrophoretic (DEP) cell separation. However, it usually limits the separation flow velocity and requires a complex multichannel fluid control system that hinders the integration of a DEP separator with other microfluidic functionalities for comprehensive biomedical applications. Here, we propose and develop a high-efficiency, sheathless particle/cell separation method without prefocusing based on flow-field-assisted DEP by combining the effects of AC electric field (E-field) and flow field (F-field). A hollow lemon-shaped electrode array is designed to generate a long-range E-field gradient in the microchannel, which can effectively induce lateral displacements of particles/cells in a continuous flow. A series of arc-shaped protrusion structures is designed along the microchannel to form a F-field, which can effectively guide the particles/cells toward the targeted E-field region without prefocusing. By tuning the E-field, two distinct modes can be realized and switched in one single device, including the sheathless separation (ShLS) and the adjustable particle mixing ratio (AMR) modes. In the ShLS mode, we have achieved the continuous separation of breast cancer cells from erythrocytes with a recovery rate of 95.5% and the separation of polystyrene particles from yeast cells with a purity of 97.1% at flow velocities over 2.59 mm/s in a 2 cm channel under optimized conditions. The AMR mode provides a strategy for controlling the mixing ratio of different particles/cells as a well-defined pretreatment method for biomedical research studies. The proposed microchip is easy to use and displays high versatility for biological and medical applications.

Symmetric Pearcey Gaussian beams.

In this Letter, a new, to the best of our knowledge, type of autofocusing and symmetric beam arisen from two quartic spectral phases is introduced in theory and experiment. The symmetric Pearcey Gaussian beam (SPGB), formed with a Gaussian term and two multiplying Pearcey integrals, processes a focusing intensity approximately 1.32 times stronger than the intensity of the symmetric Airy beam. Its four off-axis main lobes split into four bending trajectories symmetrically after focusing. The rectangular intensity distribution and the focal length of the SPGB can be adjusted by two kinds of distribution factors. Additionally, the vortex-guiding property of the beam is demonstrated by embedding an off-axis vortex into the SPGB, which can be applied in particle guiding.

Autonomous capillary microfluidic devices with constant flow rate and temperature-controlled valving.

In this paper, we report on a capillary microfluidic device with constant flow rate and temperature-triggered stop valve function. It contains a PDMS channel that was grafted by a thermo-responsive polymer poly(N-isopropylacrylamide) (PNIPAm). The channel exhibits a constant capillary filling speed. By locally increasing the temperature in the channel from 20 °C to 37 °C using a microfabricated heater, a change of the surface wettability from hydrophilic to hydrophobic is obtained creating a hydrophobic stop valve. The valve can be reopened by lowering the temperature. The device is simple to fabricate and can be used as an actuatable capillary pump operating around room temperature. To understand the constant capillary filling speed, we performed contact angle measurements, in which we found slow wetting kinetics of PNIPAm-g-PDMS surfaces at temperatures below the lower critical solution temperature (LCST) of PNIPAm and fast wetting kinetics above the LCST. We interpret this as the result of the diffusive hydration process of PNIPAm below the LCST and the absence of hydration on the hydrophobic PNIPAm thin layer above the LCST.

Novel 2D/2D BiOBr/UMOFNs direct Z-scheme photocatalyst for efficient phenol degradation.

A novel 2D/2D BiOBr/ultrathin metal-organic framework nanosheets (UMOFNs) direct Z-scheme photocatalyst was successfully synthesized by using a simple deposition-precipitation method. The photocatalytic performance was evaluated under light irradiation, which revealed that the 2D/2D BiOBr/UMOFNs Z-scheme photocatalyst exhibits higher photocatalytic degradation of phenol compared to pristine BiOBr and UMOFNs. A BiOBr/UMOFNs-40% (mass ratio for BiOBr and UMOFNs of 1:0.4) photocatalyst was found to show the best photocatalytic degradation efficiency and stability, reaching 99% phenol degradation under light irradiation of 270 min and maintaining 97% degradation after 5 recycling runs. Results obtained from a trapping experiment and electron paramagnetic resonance suggest that reactive ·OH and O2 ·- play a major role in phenol degradation. Photoluminescence and photocurrent results reveal that the excellent photocatalytic activity of the 2D/2D BiOBr/UMOFNs photocatalyst can be ascribed to the efficient separation of photogenerated electron-hole pairs through a direct Z-scheme system. This article provides a possible reference for designing Z-scheme photocatalysts by using MOFs and semiconductors for practical organic pollutant treatment.

Lithography-free synthesis of periodic, vertically-aligned, multi-walled carbon nanotube arrays.

Until now, the growth of periodic vertically aligned multi-walled carbon nanotube (VA-MWCNT) arrays was dependent on at least one lithography step during fabrication. Here, we demonstrate a lithography-free fabrication method to grow hexagonal arrays of self-standing VA-MWCNTs with tunable pitch and MWCNT size. The MWCNTs are synthesized by plasma enhanced chemical vapor deposition (PECVD) from Ni catalyst particles. Template guided dewetting of a thin Ni film on a hexagonally close-packed silica particle monolayer provides periodically distributed Ni catalyst particles as seeds for the growth of the periodic MWCNT arrays. The diameter of the silica particles directly controls the pitch of the periodic VA-MWCNT arrays from 600 nm to as small as 160 nm. The diameter and length of the individual MWCNTs can also be readily adjusted and are a function of the Ni particle size and PECVD time. This unique method of lithography-free growth of periodic VA-MWCNT arrays can be utilized for the fabrication of large-scale biomimetic materials.