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We show that the reflection interference fringe (RIF) is formed on a screen far away from the microdroplets placed on a prism-based substrate, which have low contact angles and thin droplet heights, caused by the dual convex–concave profile of the droplet, not a pure convex profile. The geometric formulation shows that the interference fringes are caused by the optical path difference when the reflected rays from the upper convex profile at the droplet–air interface interfere with reflection from the lower concave profile at oblique angles lower than the critical angle. Analytic solutions are obtained for the droplet height and the contact angle out of the fringe number and the fringe radius in RIF from the geometric formulation. Furthermore, the ray tracing simulation is conducted using the custom-designed code. The geometric formulation and the ray tracing show excellent agreement with the experimental observation in the relation between the droplet height and the fringe number and the relation between the contact angle and the fringe radius. This study is remarkable as the droplet's dual profile cannot be easily observed with the existing techniques. However, the RIF technique can effectively verify the existence of a dual profile of the microdroplets in a simple setup. In this work, the RIF technique is successfully developed as a new optical diagnostic technique to determine the microdroplet features, such as the dual profile, the height, the contact angle, the inflection point, and the precursor film thickness, by simply measuring the RIF patterns on the far-field screen. [ABSTRACT FROM AUTHOR]

Experimental findings by others suggest that OH radicals are formed in unexpected abundance on or near surfaces of 1–50 µm microdroplets comprised of pure water, but the mechanism by which these radicals are generated is not yet fully resolved. In this work, we examine two possibilities using ab initio electronic structure methods: (1) electron transfer (ET) from a microdroplet surface-bound OH− anion to a nearby H3O+ cation and (2) proton transfer (PT) from such a H3O+ cation to a nearby OH− anion. Our findings suggest that both processes are possible but only if the droplet's underlying water molecules comprising the microdroplet provide little screening of the Coulomb interaction between the anion and cation once they reach ∼10 Å of one another. In the ET event, an OH radical is formed directly; for PT, the OH formation occurs because the new O–H bond formed by the transferred proton is created at a bond length sufficiently elongated to permit homolytic cleavage. Both the ET and PT pathways predict that H atoms will also be formed. Finally, we discuss the roles played by strong local electric fields in mechanisms that have previously been proposed and that occur in our two mechanisms. [ABSTRACT FROM AUTHOR]

Effect mechanisms of the undercooling degree and the surface configuration on the ice growth characteristics were revealed under micro-droplets icing conditions. Preferential ice crystals appear firstly on the surfaces due to the randomness of icing, and obtain growth advantages to form protruding structures. Protruding structures block the incoming droplets from contacting the substrates, causing voids around the structures. The undercooling degree mainly affects the density and the growth rate of preferential ice crystals. With the increase of undercooling degree, the preferential ice crystals have higher density and growth rate, resulting in stronger growth advantage and higher porosity. The surface configuration affects the growth mode, and the ice layer grows with uniform mode, spreading mode and structure-induced mode on the aluminum, smooth Polytetrafluoroethylene (PTFE) and rough PTFE surface respectively, causing the needle-like, ridge-like and cluster-like ice crystals. The rough structures effectively improve the porosity of the ice layer, which is beneficial for optimizing the icephobic property of the materials. This paper provides important theoretical guidance for the design of subsequent icephobic materials. [ABSTRACT FROM AUTHOR]

We developed a rapid polymorphic screening approach based on contracting sessile microdroplets, which offers several advantages: (1) achieves very high supersaturation to facilitate formation of metastable forms; (2) allows systematic labeling of samples; (3) gives access to the statistical distribution of polymorphic selectivity as a function of experimental conditions; (4) ensures the formation of crystal for each droplet, addressing the problem of uncrystallized droplets in traditional microfluidics. We studied the competitive nucleation of D -mannitol polymorphs and investigated the effect of droplet volume on polymorphic selectivity. We showed that our observed polymorph distributions at different volumes are qualitatively consistent with the predictions of classical nucleation theory except for very small volumes where thermodynamic confinement or surface effects could play a substantial role. Overall, our microfluidic approach can be a promising tool not only for routine screening of pharmaceutical polymorphs in the industrial context but also in the fundamental understanding of the mechanisms underlying the competitive nucleation of polymorphs. [ABSTRACT FROM AUTHOR]

We present a smart roof that makes fragmented droplets from the impact of raindrops on superhydrophobic meshes and utilizes the droplets for agricultural spraying. This facile method transforms raindrops or waterdrops into uniform microdroplets, which can both reduce crop lodging induced by heavy rainfall, and realize uniform spraying of pesticides. [ABSTRACT FROM AUTHOR]

Targeted drug delivery system (DDS) holds exciting prospects in biomedical clinical research and drug development. However, it faces a significant challenge in achieving stable and safe targeted transportation without drug leakage while obtaining precise and controllable drug dosing with a high drug utilization rate and low side effects. Herein, an optical tweezers‐based light‐driven technique is proposed to transport and construct multi‐core/shell microdroplets enveloping drug carriers and target cells as a novel, safe, and efficient targeted DDS. Drug‐loaded microdroplets with core/shell structures are first fabricated by a new and simple injection extrusion method and then it is transported to a target cell by a dynamic optical trap with a low optical power, which ensures no drug leakage, exogenous materials, and biothermal damage are introduced during the drug delivery process. Next, precise drug dosing is realized by pushing the target cell into the drug‐loaded microdroplet under the actions of optical forces, which constructs a multi‐core/shell microdroplet structure with a pure drug environment to improve the drug action efficiency. Moreover, quantitative drug dosing with a high drug utilization rate can also achieved by controlling the sizes/number of drug droplets inside the microdroplets. This light‐driven DDS is of great interest to frontier medical research and disease treatment fields. [ABSTRACT FROM AUTHOR]

To examine if 12.5 μl timolol maleate 0.5% microdrops dispensed with the Nanodropper Adaptor provide noninferior intraocular pressure (IOP) reduction compared with conventional 28 μl drops in patients with open-angle glaucoma (OAG) and ocular hypertension (OHT). Prospective, noninferiority, parallel, multicenter, single-masked, active-controlled, randomized trial. Treatment-naïve subjects who were recently diagnosed with OAG and OHT at the Aravind Eye Care System. Both eyes of subjects received 1 commercially available drop or both eyes of subjects received 1 microdrop of timolol maleate 0.5%. We measured IOP, resting heart rate (HR), and blood pressure (BP) at baseline and 1, 2, 5, and 8 hours after timolol administration. The IOP was the primary outcome measure. Secondary outcomes were resting HR, systolic BP (sBP), and diastolic BP (dBP). Adaptor-mediated microdrops and conventional drops of timolol significantly decreased IOP compared with baseline at all timepoints. Noninferiority was established at 3 of 4 timepoints. Heart rate decreases with Nanodropper were approximately 3 beats per minute (bpm) less than with conventional drops. Timolol microdrops appear to be as effective in ocular hypotensive action as conventional drops with a slightly attenuated effect on resting HR and BP. Proprietary or commercial disclosure may be found after the references. [ABSTRACT FROM AUTHOR]

The high-speed impact of liquid microdroplets has emerged as a promising method to eliminate nanoparticle contaminants from semiconductor wafer surfaces. However, existing experimental studies have primarily focused on evaluating their own nozzles for removing particles larger than 50 nm, which does not align with the current research roadmap where the target particles' size decreases down to sub-10 nm. As it is more challenging to remove smaller particles, there is a strong need to better understand droplet's spreading behavior in relation to the detachment of particles from a surface. Nonetheless, there remains a lack of experimental evidence to validate existing models or a scarcity of numerical simulation studies, mainly due to the practical difficulties associated with single droplet experiments. Hence, in this study, we conduct a series of numerical simulations to investigate the time-dependent spreading behavior of the droplet, together with collecting local velocity data at the attached particle position. The local velocity data is then integrated to an existing model to predict the effective cleaning diameter for each impact condition. Starting from the free-fall dropwise impaction, we develop a single-microdroplet cleaning system by minimizing the number of sprayed droplets and capturing their behavior using a high-speed camera (HSC), with aims of validating the model predictions and numerical simulations. Finally, we provide a contour plot for a prior prediction of the effective cleaning diameter from the impaction conditions of microdroplets. Copyright © 2024 American Association for Aerosol Research [ABSTRACT FROM AUTHOR]

Membraneless coacervate microdroplets have long been proposed as model protocells as they can grow, divide, and concentrate RNA by natural partitioning. However, the rapid exchange of RNA between these compartments, along with their rapid fusion, both within minutes, means that individual droplets would be unable to maintain their separate genetic identities. Hence, Darwinian evolution would not be possible, and the population would be vulnerable to collapse due to the rapid spread of parasitic RNAs. In this study, we show that distilled water, mimicking rain/freshwater, leads to the formation of electrostatic crosslinks on the interface of coacervate droplets that not only suppress droplet fusion indefinitely but also allow the spatiotemporal compartmentalization of RNA on a timescale of days depending on the length and structure of RNA. We suggest that these nonfusing membraneless droplets could potentially act as protocells with the capacity to evolve compartmentalized ribozymes in prebiotic environments. [ABSTRACT FROM AUTHOR]

The ability of analytical strategies to detect and positively identify molecules under extremely dilute conditions is important for the growth and expansion of analytical techniques and instrumentation. At present, few measurement science techniques can robustly approach the measurement of just a few thousand molecules. Here, we present an electrochemical platform for the detection and positive identification of fewer than 1000 molecules of decamethylferrocene ((Cp*)2FeII). We achieve this remarkable detection threshold by trapping (Cp*)2FeII in a 1,2-dichloroethane microdroplet, which is allowed to dissolve into an aqueous continuous phase while on a gold microelectrode (radius ∼6.25 μm). Because electrochemistry is not sensitive enough to observe the charge of less than 1000 molecules, we dissolved μM amounts hexacyanoferrate(III) in the aqueous continuous phase. The biphasic reaction between hexacyanoferrate(III) and Cp2*(Fe)II allows for a feedback loop when the microelectrode is biased sufficiently negative to reduce Cp2*(Fe)III. This feedback loop, a typical EC′ catalytic mechanism, amplifies the electrochemical signal of Cp2*(Fe)II when the droplet is of small enough dimensions for feedback to occur. Our results demonstrate that clever biphasic reactions can be coupled with dissolving microdroplets to access extremely low limits of quantitation in electroanalysis. [ABSTRACT FROM AUTHOR]

We report a novel method to conduct heterogeneous reactions using aqueous-ionic liquid Janus microdroplets as a series of isolated bi-phasic microreactors where AgCl@polyaniline core–shell nanoparticles are successfully synthesized accompanied by polyaniline nano-needles, and enhanced visualization of reaction progression through the color changes in Janus droplets is achieved. [ABSTRACT FROM AUTHOR]

Polymer microparticle synthesis based on the surface‐templated method is a simple and environmentally friendly method to produce various microparticles. Unique particles with different compositions can be fabricated by simply annealing a polymer on a liquid‐repellent surface. However, there are hurdles to producing particles of homogeneous sizes with large quantities and varying the shape of particles. Here, a new approach to synthesizing multiple polymer microparticles using micropatterns with wettability contrast is presented. Polymer microparticles are formed in two steps. First, a layer of poly(sodium‐4‐styrenesulfonate) is deposited on the hydrophilic regions by dipping and withdrawing this micropattern from a polymer solution, and an array of microdroplets is formed. A dewetting‐inducing layer on the pattern is introduced, and then target polymer patches are sequentially generated on it. By annealing over Tg, the contact line of the target polymer patch is freely receded, creating a particle form. The size and shape of the microparticle can be controlled by varying the micropatterns. In addition, it is demonstrated that microparticles made of polymer blends or polymer/nanoparticle composite are easily produced. This versatile method offers the potential of surface‐templated synthesis to tailor polymer microparticles with different sizes, shapes, and functionalities in various research and applications. [ABSTRACT FROM AUTHOR]

Droplet sorting and enrichment, as a prominent field within microfluidic technology, represent a pivotal stage in the manipulation of droplets and particles. In recent times, droplet sorting methods based on lab-on-disk (LOD) have garnered significant interest among researchers for their inherent merits, including high throughput, ease of operation, seamless device integration, and independence from supplementary driving forces. This study introduces a centrifugal force-driven microfluidic chip comprising spiral microchannels. The chip incorporates microhole arrays along the sidewall of the spiral channels, enabling size-based sorting and enrichment of microdroplets under the influence of multiple forces. Firstly, a comparative analysis was performed to assess the influence of the separation port structure and rotational speed on efficiency, and a mechanical modeling approach was employed to conduct kinetic analyses of droplet behavior during instantaneous separation. Those findings demonstrated a good agreement with the experimental results at ω < 100 rpm. Subsequently, sorting experiments on homogeneous droplets indicated that repetitive sorting could increase the recovery ratios, RT(α), of high-concentration droplets (20.7%) from 35.3% to over 80%. We also conducted a sorting experiment on three-component homogeneous-phase emulsions using a serially connected chip array, and the sorting throughput was 0.58 mL min−1. As a result, the RT(α) for 60 and 160 μm droplets were 99.4% and 88.9%, respectively. Lastly, we conducted elution experiments and dual-sample sorting on a single chip, and the fluorescence results demonstrated that this study provided an efficient and non-cross-contaminating sorting method for non-homogenous phase multi-sample microreactor units. [ABSTRACT FROM AUTHOR]

Droplet evaporation and dissolution phenomena are pervasive in both natural and artificial systems, playing crucial roles in various applications. Understanding the intricate processes involved in the evaporation and dissolution of sessile droplets is of paramount importance for applications such as inkjet printing, surface coating, and nanoparticle deposition, etc. In this study, we present a demonstration of electrochemical investigation of the dissolution behaviour in sub-nL droplets down to sub-pL volume. Droplets on an electrode have been studied for decades in the field of electrochemistry to understand the phase transfer of ions at the oil–water interface, accelerated reaction rates in microdroplets, etc. However, the impact of microdroplet dissolution on the redox activity of confined molecules within the droplet has not been explored previously. As a proof-of-principle, we examine the dissolution kinetics of 1,2-dichloroethane droplets (DCE) spiked with 155 μM decamethylferrocene within an aqueous phase on an ultramicroelectrode (r = 6.3 μm). The aqueous phase serves as an infinite sink, enabling the dissolution of DCE droplets while also facilitating convenient electrical contact with the reference/counter electrode (Ag/AgCl 1 M KCl). Through comprehensive voltammetric analysis, we unravel the impact of droplet dissolution on electrochemical response as the droplet reaches minuscule volumes. We validate our experimental findings by finite element modelling, which shows deviations from the experimental results as the droplet accesses negligible volumes, suggesting the presence of complex dissolution modes. [ABSTRACT FROM AUTHOR]

The interaction of perfluorinated molecules, also known as "forever chemicals" due to their pervasiveness, with their environment remains an important yet poorly understood topic. In this work, the self‐assembly of perfluorinated molecules with multivalent hosts, pillar‐[5]‐arenes, is investigated. It is found that perfluoroalkyl diacids and pillar‐[5]‐arenes rapidly and strongly complex with each other at aqueous interfaces, forming solid interfacially templated films. Their complexation is shown to be driven primarily by fluorophilic aggregation and assisted by electrostatic interactions, as supported by the crystal structure of the complexes, and leads to the formation of quasi‐2D phase‐separated films. This self‐assembly process can be further manipulated using aqueous two‐phase system microdroplets, enabling the controlled formation of 3D micro‐scaffolds. [ABSTRACT FROM AUTHOR]

The efficient reduction of CO2 into valuable products is a challenging task in an international context marked by the climate change crisis and the need to move away from fossil fuels. Recently, the use of water microdroplets has emerged as an interesting reaction media where many redox processes which do not occur in conventional solutions take place spontaneously. Indeed, several experimental studies in microdroplets have already been devoted to study the reduction of CO2 with promising results. The increased reactivity in microdroplets is thought to be linked to unique electrostatic solvation effects at the air‐water interface. In the present work, we report a theoretical investigation on this issue for CO2 using first‐principles molecular dynamics simulations. We show that CO2 is stabilized at the interface, where it can accumulate, and that compared to bulk water solution, its electron capture ability is larger. Our results suggest that reduction of CO2 might be easier in interface‐rich systems such as water microdroplets, which is in line with early experimental data and indicate directions for future laboratory studies. The effect of other relevant factors which could play a role in CO2 reduction potential is discussed. [ABSTRACT FROM AUTHOR]

Traditional circuit board fabrication schemes are not directly applicable to the production of flexible, multi‐material circuits. This article reports a technique, microfluidic directed material patterning, which combines soft microfluidic stamps and low‐temperature solution‐phase deposition to generate multi‐material circuits on flexible, non‐planar polymeric supports. Specifically, metallic and semiconductive traces are combined on commodity plastic films to yield functional photosensitive circuits that can be used in the spectrophotometric detection and concentration measurement of microdroplets on 3D “e‐plates.” The photoresistive material cadmium sulfide is used in these circuits because it is suitable for visible light detection and it can be deposited directly from aqueous solutions following established bath deposition procedures. This method can produce colorimetric devices capable of quantifying micromolar concentrations of Allura Red in microdroplets of Kool‐Aid. This technique presents the opportunity for producing single‐use or low‐use disposable/recyclable devices for flexible 3D sensors and detectors following a convenient, low‐waste fabrication scheme. The general capabilities of this approach, in terms of substrate geometry and device layout (e.g., the number, area, and pattern of photoresistive elements), can be applied to the design and manufacture of more intricate, multiplexed devices supportive of advanced and/or specialized functions that go beyond those reported in this initial demonstration. [ABSTRACT FROM AUTHOR]

Recent advances in composite hydrogels achieve material enhancement or specialized stimuli‐responsive functionalities by pairing with a functional filler. Liquid metals (LM) offer a unique combination of chemical, electrical, and mechanical properties that show great potential in hydrogel composites. Polymerization of hydrogels with LM microdroplets as initiators is a particularly interesting phenomenon that remains in its early stage of development. In this work, an LM‐hydrogel composite is introduced, in which LM microdroplets dispersed inside the hydrogel matrix have dual functions as a polymerization initiator for a polyacrylic acid‐poly vinyl alcohol (PAA/PVA) network and, once polymerized, as passive inclusion to influence its material and stimuli‐responsive characteristics. It is demonstrated that LM microdroplets enable ultra‐fast polymerization in ≈1 min, compared to several hours by conventional polymerization techniques. The results show several mechanical enhancements to the PAA/PVA hydrogels with LM‐initiated polymerization. It is found that LM ratios strongly influence stimuli‐responsive behaviors in the hydrogels, including swelling and ionic bending, where higher LM ratios are found to enhance ionic actuation performance. The dual roles of LM in this composite are analyzed using the experimental characterization results. These LM‐hydrogel composites, which are biocompatible, open up new opportunities in future soft robotics and biomedical applications. [ABSTRACT FROM AUTHOR]

Liquid metal (LM) droplet‐embedded polymer composites with exceptional thermal, electrical, and mechanical characteristics are attractive for applications in soft electronics and thermal management. Generally, a high volume fraction of LMs is required for desirable thermal and electrical properties, and thus recycling of LMs is favorable and cost effective. However, recycling LMs from composites remains a formidable challenge because the LM droplets are typically dispersed into a permanent covalently crosslinked polymer matrix. Here, a facile synthesis of LM‐polymer composites with high electrical conductivity (1800 S cm−1), high stretchability (1400% tensile strain), as well as degradability and recyclability is reported. The composite comprises a poly(2‐hydroxyethyl acrylate) hydrogel that is physically crosslinked by LM nanodroplets as a polymer matrix and either LM microdroplets or silver microflakes as a conductive filler. A postdrying process improves the mechanical performance of the composite while creating percolating pathways via the rearrangement of the conductive fillers, imparting high electrical conductivity to the composite. Moreover, the composites are readily degraded and dissolved in aqueous alkali solutions at room temperature thanks to the reactive nature of LM crosslinks, enabling high recycling efficiency of ≈80% and 95% for composites with LM microdroplets and silver microflakes as conductive fillers, respectively. [ABSTRACT FROM AUTHOR]

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Yeast plays a significant role in a variety of fields. In particular, it is extensively used as a model organism in genetics and cellular biology studies, and is employed in the production of vaccines, pharmaceuticals, and biofuels. Traditional "bulk"-based studies on yeast growth often overlook cellular variability, emphasizing the need for single-cell analysis. Micro-droplets, tiny liquid droplets with high surface-area-to-volume ratios, offer a promising platform for investigating single or a small number of cells, allowing precise control and monitoring of individual cell behaviors. Microfluidic devices, which facilitate the generation of micro-droplets, are advantageous due to their reduced volume requirements and ability to mimic in vivo micro-environments. This study introduces a custom-designed microfluidic device to encapsulate yeasts in micro-droplets under various conditions in a parallel manner. The results reveal that optimal glucose concentrations promoted yeast growth while cycloheximide and Cu2+ ions inhibited it. This platform enhances yeast cultivation strategies and holds potential for high-throughput single-cell investigations in more complex organisms. [ABSTRACT FROM AUTHOR]

Overcoming the oxygen diffusion limit of approximately 200 µm remains one of the most significant and intractable challenges to be overcome in tissue engineering. The fabrication of hydrogel microtissues and their assembly into larger structures may provide a solution, though these constructs are not without their own drawbacks; namely, these hydrogels are rapidly degraded in vivo, and cells delivered via microtissues are quickly expelled from the area of action. Here, we report the development of an easily customized protocol for creating a protective, biocompatible hydrogel barrier around microtissues. We show that calcium carbonate nanoparticles embedded within an ECM-based microtissue diffuse outwards and, when then exposed to a solution of alginate, can be used to generate a coated layer around the tissue. We further show that this technique can be fine-tuned by adjusting numerous parameters, granting us full control over the thickness of the hydrogel coating layer. The microtissues' protective hydrogel functioned as hypothesized in both in vitro and in vivo testing by preventing the cells inside the tissue from escaping and protecting the microdroplets against external degradation. This technology may provide microtissues with customized properties for use as sources of regenerative therapies. [ABSTRACT FROM AUTHOR]

Nucleation, the birth of a stable cluster from a disorder, is inherently stochastic. Yet up to date, there are no quantitative studies on NaCl nucleation that accounts for its stochastic nature. Here, we report the first stochastic treatment of NaCl-water nucleation kinetics. Using a recently developed microfluidic system and evaporation model, our measured interfacial energies extracted from a modified Poisson distribution of nucleation time show an excellent agreement with theoretical predictions. Furthermore, analysis of nucleation parameters in 0.5, 1.5, and 5.5 pl microdroplets reveals an interesting interplay between confinement effects and shifting of nucleation mechanisms. Overall, our findings highlight the need to treat nucleation stochastically rather than deterministically to bridge the gap between theory and experiment. [ABSTRACT FROM AUTHOR]

We present a catalyst‐free route for the reduction of carbon dioxide integrated with the formation of a carbon‐carbon bond at the air/water interface of negatively charged aqueous microdroplets, at ambient temperature. The reactions proceed through carbanion generation at the α‐carbon of a ketone followed by nucleophilic addition to CO2. Online mass spectrometry reveals that the product is an α‐ketoacid. Several factors, such as the concentration of the reagents, pressure of CO2 gas, and distance traveled by the droplets, control the kinetics of the reaction. Theoretical calculations suggest that water in the microdroplets facilitates this unusual chemistry. Furthermore, such a microdroplet strategy has been extended to seven different ketones. This work demonstrates a green pathway for the reduction of CO2 to useful carboxylated organic products. [ABSTRACT FROM AUTHOR]

This report presents liquid metal-based infrared-modulating materials and systems with multiple modes to regulate the infrared reflection. Inspired by the brightness adjustment in chameleon skin, shape-morphing liquid metal droplets in silicone elastomer (Ecoflex) matrix are used to resemble the dispersed "melanophores". In the system, Ecoflex acts as hormone to drive the deformation of liquid metal droplets. Both total and specular reflectance-based infrared camouflage are achieved. Typically, the total and specular reflectances show change of ~44.8% and 61.2%, respectively, which are among the highest values reported for infrared camouflage. Programmable infrared encoding/decoding is explored by adjusting the concentration of liquid metal and applying areal strains. By introducing alloys with different melting points, temperature-dependent infrared painting/writing can be achieved. Furthermore, the multi-layered structure of infrared-modulating system is designed, where the liquid metal-based infrared modulating materials are integrated with an evaporated metallic film for enhanced performance of such system. Liquid metal-based infrared-modulating materials and systems have been developed to regulate the infrared reflection with multiple modes, which can be used for infrared camouflage, programmable infrared encryption, and infrared painting/writing. [ABSTRACT FROM AUTHOR]

[Display omitted] Water wetting induced corrosion is the core issue for uncovering the corrosion mechanism in multiphase flow environments, relevant to many industrial applications. Here, we experimentally investigated the dynamic failure of an oil film attached on the pre-wetted model surfaces by the electrochemical current detection using an "Alternate Wetting Cell" and the direct visualization of near-wall fluid states. The oil pre-wetted surface performed a superior corrosion mitigation efficiency, exhibiting a protective oil film with a duration time at least 5 times longer than the water pre-wetted surface. It confirms that the oil film rupture is a combined process of the local penetration and pinning of micro-droplets and the phase redistribution of the near-wall fluids. Corrosion finally initiates and propagates on the surface once the droplets pin there or damage the oil film. The result suggests new control strategies for materials corrosion in complex systems by surface modification and fluid management. [ABSTRACT FROM AUTHOR]

Organic-inorganic interactions regulate the dynamics of hydrocarbons, water, minerals, CO2, and H2 in thermal rocks, yet their initiation remains debated. To address this, we conducted isotope-tagged and in-situ visual thermal experiments. Isotope-tagged studies revealed extensive H/O transfers in hydrous n-C20H42-H2O-feldspar systems. Visual experiments observed water microdroplets forming at 150–165 °C in oil phases near the water-oil interface without surfactants, persisting until complete miscibility above 350 °C. Electron paramagnetic resonance (EPR) detected hydroxyl free radicals concurrent with microdroplet formation. Here we propose a two-fold mechanism: water-derived and n-C20H42-derived free radicals drive interactions with organic species, while water-derived and mineral-derived ions trigger mineral interactions. These processes, facilitated by microdroplets and bulk water, blur boundaries between organic and inorganic species, enabling extensive interactions and mass transfer. Our findings redefine microscopic interplays between organic and inorganic components, offering insights into diagenetic and hydrous-metamorphic processes, and mass transfer cycles in deep basins and subduction zones. At elevated temperatures, water microdroplets emerge near oil-water interfaces, functioning as tiny geochemical reactors that initiate interactions and mass transfer among organic and inorganic components in thermal geosystems. [ABSTRACT FROM AUTHOR]

The cell membrane not only serves as the boundary between the cell's interior and the external environment but also plays a crucial role in regulating fundamental cellular behaviours. Interfacial membranization of membraneless coacervates, formed through liquid-liquid phase separation (LLPS), represents a reliable approach to constructing hierarchical cell-like entities known as protocells. In this study, we demonstrate the capability to modulate the interfacial membrane fluidity and thickness of dextran-bound coacervate protocells by adjusting the molecular weight of dextran or utilizing dextranase-catalyzed hydrolysis. This modulation allows for rational control over colloidal stability, interfacial molecular transport and cell-protocell interactions. Our work opens a new avenue for surface engineering of coacervate protocells, enabling the establishment of cell-mimicking structures and behaviours. Membranization of coacervate microdroplets can stabilize coacervates and enable the construction of hierarchical protocells by using various interfacial layers. Here, the authors demonstrate the modulation of interfacial membrane fluidity and thickness of dextran-bound coacervate protocells by adjusting the molecular weight of dextran or through enzymatic hydrolysis, achieving control over colloidal stability, interfacial molecular transport and cell-protocell interactions. [ABSTRACT FROM AUTHOR]

Due to their high surface area and low weight, silica aerogels are ideally suited for several uses, including drug delivery, catalysis, and insulation. Oil–water–oil (OWO) double emulsion is a simple and regulated technique for encasing a volatile oil phase in a silica shell to produce hollow silica (SiO2) aerogel particles by using hydrophilic and hydrophobic emulsifiers. In this study, the oil–water–oil (OWO) double emulsion method was implemented to synthesize surface-modified hollow silica (SiO2) aerogel particles in a facile and effective way. This investigation mainly focused on the influence of the N-hexane-to-water glass (OW) ratio (r) in the first emulsion, silica (water glass) content concentration (x), and surfactant concentration (s) variations. Furthermore, surface modification techniques were utilized to customize the aerogel's characteristics. The X-ray diffraction (XRD) patterns showed no imprints of impurities except SiO2. Scanning electron microscopy (SEM) and transmission electron microscopy (TEM) images highlight the hollow microstructure of silica particles. Zeta potential was used to determine particle size analysis of hollow silica aerogel particles. The oil–water–oil (OWO) double emulsion approach was successfully employed to synthesize surface-modified hollow silica (SiO2) aerogel particles, providing precise control over the particle characteristics. By the influence of the optimization condition, this approach improves the aerogel's potential applications in drug delivery, catalysis, and insulation by enabling surface modifications. [ABSTRACT FROM AUTHOR]

In this work, we show that particles of common minerals break down spontaneously to form nanoparticles charged water microdroplets within milliseconds. We transformed micron-sized natural minerals like quartz and ruby into 5- to 10-nanometer particles when integrated into aqueous microdroplets generated via electrospray. We deposited the droplets on a substrate, which allowed nanoparticle characterization. We determined through simulations that quartz undergoes proton-induced slip, especially when reduced in size and exposed to an electric field. This leads to particle scission and the formation of silicate fragments, which we confirmed with mass spectrometry. This rapid weathering process may be important for soil formation, given the prevalence of charged aerosols in the atmosphere. [ABSTRACT FROM AUTHOR]

Gas-liquid-solid catalytic reactions are widespread in nature and man-made technologies. Recently, the exceptional reactivity observed on (electro)sprayed microdroplets, in comparison to bulk gas-liquid systems, has attracted the attention of researchers. In this perspective, we compile possible strategies to engineer catalytically active gas-liquid-(solid) interfaces based on membrane contactors, microdroplets, micromarbles, microbubbles, and microfoams to produce commodity chemicals such as hydrogen peroxide, ammonia, and formic acid. In particular, particle-stabilized microfoams, with superior upscaling capacity, emerge as a promising and versatile platform to conceive high-performing (catalytic) gas-liquid-(solid) nanoreactors. Gas-liquid-(solid) nanoreactors could circumvent current limitations of state-of-the-art multiphase reactors (e.g., stirred tanks, trickle beds, and bubble columns) suffering from poor gas solubility and mass transfer resistances and access gas-liquid- (solid) reactors with lower cost and carbon footprint. [ABSTRACT FROM AUTHOR]

The ability to transfer microdroplets between fluid phases offers numerous advantages in various fields. This study focuses on the stability and morphology of a sessile oil microdropletduring the transfer from underwater to air. A distinct transition in microdroplet dynamics is observed, characterized by a shift from a scenario dominated by Marangoni forces to one dominated by capillary forces. In the former regime, the oil microdroplets spread in response to the contact between the water‐air interface and the water‐oil interface. The spreading distance follows a power law relationship of t3/4, reflecting the balance between Marangoni forces and viscous forces. On the other hand, in the capillarity‐dominated regime, the oil microdroplets remain stable at the contact line and after being transferred into the air. The crossover between these two regimes is identified in the parameter space defined by three factors: the approaching velocity of the solid‐water‐air contact line (vcl), the radius of the oil microdroplet (ro), and the radius of the water drop (rw). Furthermore, how to use the four‐phase contact line for shaping oil microdroplets is demonstrated using a full liquid process by the contact line lithography. [ABSTRACT FROM AUTHOR]

Recently, spICP-MS analyses of microplastics have demonstrated that the detection capabilities of ICP-MS are sufficient to determine the size and composition of such materials. However, solution nebulization or microdroplet generation limits the sizes of droplets, microparticles, or cells that can be efficiently introduced into commonly used horizontal ICP-MS configurations. Therefore, we introduced the development of a downward-pointing ICP coupled to a time-of-flight mass spectrometer (ICP-TOFMS), which enables quantitative transport of large microdroplets (diameters up to 90 µm) into the ICP. Here, we report the capabilities of downward ICP-TOFMS for the quantitative analysis of single cells and microplastic particles. For calibration of element mass amount per particle or cell, microdroplets (70 µm diameter) composed of multielement solutions were measured by ICP-TOFMS. Microplastic beads (polystyrene) and spleenocyte cells were then also embedded in microdroplets and measured by ICP-TOFMS with ion optics optimized to determine the signals from 12C+ and other isotopes of interest, including 140Ce, 153Eu, 165Ho, and 175Lu from the REE beads and 31P for the cells. The results achieved using the prototype instrument of a vertical downward-pointing ICP-TOFMS demonstrate that such a plasma configuration is well suited to analyze microplastics and single cells. For single microbead and cell analyses, the critical mass for carbon was 4.8 pg, and the mean determined carbon mass amounts were 14 and 23 pg, respectively. For the microbead analysis, the detected carbon mass corresponds to a particle diameter of 2.93 ± 0.24 µm, which is consistent with the scanning (transmission) electron microscopy–determined diameter of 2.97 ± 0.04 µm. Furthermore, in the analysis of spleenocyte cells, carbon and phosphorus masses were determined to be correlated. [ABSTRACT FROM AUTHOR]

We propose a novel mechanism for visualizing the chirality of compounds in solution using a vertical contact‐separation process (VCSP) of liquid crystal micro‐droplets (LCμDs). By employing the VCSP between target micro‐droplets and sensor LCμDs, the chiral compounds initially introduced in the target micro‐droplets diffuse into coalescent micro‐droplets. After the VCSP, we observed a wavelength shift in the selective reflection from the sensor LCμDs, allowing us to visualize the chirality present in the target micro‐droplets. To quantitatively analyze the wavelength shift of the selective reflection, we utilized reflective spectroscopic techniques. Our findings demonstrate that the chirality sensing mechanism achieves a detection accuracy of 10 μg. Moreover, this chiral sensing mechanism can be effectively applied to two‐dimensional micro‐droplet array systems. © 2023 Institute of Electrical Engineer of Japan and Wiley Periodicals LLC. [ABSTRACT FROM AUTHOR]

This study delves into the dynamics of generating microdroplets by impacting a droplet onto a micropore on superhydrophobic copper substrates. It identifies the necessary impact velocities for single microdroplet formation for each micropore and characterizes microdroplet size in relation to micropore diameter. The results underscore the significant role of viscosity, especially as the diameter of the micropore decreases. For micropores measuring 400 μm, an increase in viscosity up to 8 cP does not alter the critical impact velocities, while smaller diameters of 50 and 100 μm see a notable change in critical velocities with even minor increases in viscosity. Remarkably, the diameter of the microdroplet remains consistent regardless of changes in the liquid viscosity or impact velocity. This research showcases two practical uses of single microdroplets: printing on paper and fabricating microbeads. The insights gained from these findings pave the way for advancements in printing technology and microfabrication techniques. [ABSTRACT FROM AUTHOR]

In this study, the mechanisms of jet atomization were analyzed based on a frequency analysis of atomization sounds in the audible range (∼20 kHz). Jet atomization is a two-dimensional, high-speed atomization using a diaphragm, and interesting acoustic signals and atomization phenomena were detected on hydrophobic and hydrophilic diaphragms. The hydrophilic diaphragm strongly interacted and resonated with the surface wave, resulting in symmetrical jet atomization relative to the diaphragm. The resonance between the diaphragm and the surface wave was supported by a calculation of the eigenfrequency of the diaphragm and the coincidence of the droplet diameters as calculated from Lang's equation. Notably, the diaphragm excited by the ultrasonic transducer acted as a new transducer vibrating perpendicular to the transducer. As a result, when the diaphragm and the surface wave were in resonance at 2.4 MHz, a symmetrical two-dimensional high-speed jet atomization was generated in the direction perpendicular to the transducer's vibration direction. This study also revealed that the atomization state can be determined based on the acoustic analysis. This acoustic analysis of atomization sounds can be applied in more advanced atomization control, such as for providing uniform dispersions of droplets containing DNA, drugs, or microplastics. [ABSTRACT FROM AUTHOR]

Barcodes are useful for identifying objects across time, space, and information modalities. However, materializing and decoding optical and multimodal barcodes on microscopic objects remains difficult despite the increasing need for multiplexed cell analysis. Here, a computational design of randomly combinatorial is presented, yet decodable barcodes in microdroplets. The design is based on a novel Real2Sim2Real framework: it first collects experimental images of optically distinct microparticles, then simulates massive combinatorial images by randomly assembling the imaged particles to train a neural network‐based decoder. It is demonstrated that the decoder, even though trained via simulation, accurately identifies the randomly assembled particles in real hydrogel microdroplets. It also shows that the microdroplets with an additional DNA barcoding functionality are applicable to individually link independently measured microscopic images and transcriptome profiles of pooled single cells. [ABSTRACT FROM AUTHOR]

Exploration of the unique chemical properties of interfaces can unlock new understanding. A striking example is the finding of accelerated reactions, particularly spontaneous oxidation reactions, that occur without assistance of catalysts or external oxidants at the air interface of both aqueous and organic solutions (provided they contain some water). This finding opened a new area of interfacial chemistry but also caused heated debate regarding the primary chemical species responsible for the observed oxidation. An overview of the literature covering oxidation in microdroplets with air interfaces is provided, together with a critical examination of previous findings and hypotheses. The water radical cation/radical anion pair, formed spontaneously and responsible for the electric field at or near the droplet/air interface, is suggested to constitute the primary redox species. Mechanisms of accelerated microdroplet reactions are critically discussed and it is shown that hydroxyl radical/hydrogen peroxide formation in microdroplets does not require that these species be the primary oxidant. Instead, we suggest that hydroxyl radical and hydrogen peroxide are the products of water radical cation decay in water. The importance of microdroplet chemistry in the prebiotic environment is sketched briefly and the role of partial solvation in reaction acceleration is noted. [ABSTRACT FROM AUTHOR]

Microdroplets are a class of soft matter that has been extensively employed for chemical, biochemical, and industrial applications. However, fabricating microdroplets with largely controllable contact-area shape and apparent contact angle, a key prerequisite for their applications, is still a challenge. Here, by engineering a type of surface with homocentric closed-loop microwalls/microchannels, we can achieve facile size, shape, and contact-angle tunability of microdroplets on the textured surfaces by design. More importantly, this class of surface topologies (with universal genus value = 1) allows us to reveal that the conventional Gibbs equation (widely used for assessing the edge effect on the apparent contact angle of macrodroplets) seems no longer applicable for water microdroplets or nanodroplets (evidenced by independent molecular dynamics simulations). Notably, for the flat surface with the intrinsic contact angle ~0°, we find that the critical contact angle on the microtextured counterparts (at edge angle 90°) can be as large as >130°, rather than 90° according to the Gibbs equation. Experiments show that the breakdown of the Gibbs equation occurs for microdroplets of different types of liquids including alcohol and hydrocarbon oils. Overall, the microtextured surface design and topological wetting states not only offer opportunities for diverse applications of microdroplets such as controllable chemical reactions and low-cost circuit fabrications but also provide testbeds for advancing the fundamental surface science of wetting beyond the Gibbs equation. [ABSTRACT FROM AUTHOR]

This project presents a quantitative detection method to identify raccoon‐derived ingredient adulteration in sausage products. The specific copy gene of the raccoon was selected as the target gene. According to the specificity of its primer and probe, the quantitative detection method of raccoon microdrops by droplet digital PCR was established. In addition, the accuracy of the proposed method was verified by artificially mixed samples, and the applicability of this method was tested based on the commercially available products. The experimental results indicate that the raccoon mass (M) and raccoon‐extracted DNA concentration have a good linear relationship when the sample content is 5–100 mg, and there is also a significant linear relationship between DNA content and DNA copy number (C) with R2 =.9982. Therefore, using DNA concentration as the median signal, the conversion equation between raw raccoon mass (M) and DNA copy number (C) could be obtained as follows: M = (C + 177.403)/16.954. The detection of artificially mixed samples and commercial samples shows that the method is accurate and suitable for quantitative adulteration detection of various sausage products in the market. [ABSTRACT FROM AUTHOR]

Tiered micro‐nanogradient structures with custom‐tailored profiles and dimensions can be fabricated by the anisotropic electrochemical anodization of aluminum, where the micro and nanostructures are simultaneously formed. The microgradient structures can be sculpted by the chronological and spatial order of polymer masking followed by step anodization; the nanostructures can be controlled by electrochemical conditions in step anodization. Water spatial distribution and directional transportation abilities of the exemplified micro‐nanogradient structures (i.e., tiered micro symmetric circular structure, microasymmetric circular structure, and microrectangular step structure which are all integrated with nanotip‐capped nanopore structure) are studied under the fogging condition. It is found that despite the directional self‐jumping of the microdroplets caused by the cooperation of asymmetric structure and wind blowing, microdroplets can also be quickly gathered on the topper tier of the gradient structures to form large droplets and then roll away along the descending direction of the structures (also wind blowing direction), which sweep the microdroplets they passed by. These tiered micro‐nanogradient structures not only have potentials to become high efficiency fog collector but also could be a platform for the preparation of tiered micro‐nanogradient structures of various materials with advanced functions. [ABSTRACT FROM AUTHOR]

Electron emission from microdroplets subjected to a distortion in its spherical shape by a pre-pulse is studied, especially to decipher the role of chirp in the laser pulse. While there are some noticeable differences in the spectral shape with sign of the chirp, the change in the average electron energy is small. Increase in the pulse width diminishes the electron emission propensity and also the average electron energy. Analytical formalism on the two-plasmon decay instability identified to be responsible for the electron emission provides insight to explain the measurements. Electron emission computed by 2D particle-in-cell simulations for these experiments compares very well with the measurements. [ABSTRACT FROM AUTHOR]

Microdroplet resonators provide an excellent tool for optical studies of water, but water microdroplets are difficult to maintain outside a carefully controlled environment. We present a method for maintaining a water microdroplet resonator on a 3D-printed hydrophobic surface in an ambient environment. The droplet is maintained through a passive microfluidic system that supplies water to the droplet through a vertical channel at a rate equivalent to its evaporation. In this manner, we are able to create and passively maintain water microdroplet resonators with quality factors as high as  3 × 10 8 . [ABSTRACT FROM AUTHOR]

Recent reports have detailed the striking observation that electroactive molecules, such as hydrogen peroxide (H2O2) and radical water species (H2O.+/H2O.-), are spontaneously produced in aqueous microdroplets. Stochastic electrochemistry allows one to study reactions in real-time occurring inside subfemtoliter droplets, one droplet at a time, when a microdroplet irreversibly adsorbs to an ultramicroelectrode surface (radius ~ 5 µm). Here, we use stochastic electrochemistry to probe the formation of hydrogen peroxide (H2O2) in single aqueous microdroplets suspended in 1,2-dichloroethane. The oxidation of H2O2 at alkaline pH (11.5) differs from near-neutral conditions (6.4), allowing us to create a digital, turn-off sensing modality for the presence of H2O2. Further, we show that the stochastic electrochemical signal is highest at the mass transfer limitation of the H2O2 couple and is dampened when the potential nears the formal potential. We validate these results by showing that the addition of a H2O2 selective probe, luminol, decreases the stochastic electrochemical response at alkaline pH (11.5). Our results support the observation that H2O2 is generated in water microdroplets at concentrations of ~100 s of µM. [ABSTRACT FROM AUTHOR]

Water microdroplets (7 to 11 µm average diameter, depending on flow rate) are sprayed in a closed chamber at ambient temperature, whose relative humidity (RH) is controlled. The resulting concentration of ROS (reactive oxygen species) formed in the microdroplets, measured by the amount of hydrogen peroxide (H2O2), is determined by nuclear magnetic resonance (NMR) and by spectrofluorimetric assays after the droplets are collected. The results are found to agree closely with one another. In addition, hydrated hydroxyl radical cations (•OH-H3O+) are recorded from the droplets using mass spectrometry and superoxide radical anions (•O2 -) and hydroxyl radicals (•OH) by electron paramagnetic resonance spectroscopy. As the RH varies from 15 to 95%, the concentration of H2O2 shows a marked rise by a factor of about 3.5 in going from 15 to 50%, then levels off. By replacing the H2O of the sprayed water with deuterium oxide (D2O) but keeping the gas surrounding droplets with H2O, mass spectrometric analysis of the hydrated hydroxyl radical cations demonstrates that the water in the air plays a dominant role in producing H2O2 and other ROS, which accounts for the variation with RH. As RH increases, the droplet evaporation rate decreases. These two facts help us understand why viruses in droplets both survive better at low RH values, as found in indoor air in the wintertime, and are disinfected more effectively at higher RH values, as found in indoor air in the summertime, thus explaining the recognized seasonality of airborne viral infections. [ABSTRACT FROM AUTHOR]

Complex mixtures are typically analyzed by chromatographic separation followed by mass spectrometry. Two‐dimensional tandem mass spectrometry (2D MS/MS) may eliminate the need for separation and therefore significantly reduce analysis time while expanding the information space by recording the intensities of all fragment ions generated from all trapped precursor ions. Additional chemical specificity can be provided by using chemical derivatization. In this study phenolic compounds are identified after triazole click derivatization by the observation of two diagnostic features in the 2D MS/MS data domain, a mass shift of 175 Da on the precursor ion axis and a neutral loss (NL) of 119 Da. Additional NL transitions were highly correlated with particular substituents including carbonyl, ester, amino, and alkyl/phenyl groups. Substituent position information was also easily diagnosed. The derivatization reactions are accelerated in the charged electrosprayed microdroplets. Using this method, members of this single class of compounds can be identified within 1–2 minutes while structural information on the individual compounds is acquired simultaneously. [ABSTRACT FROM AUTHOR]

Micro Electrodes Dot Array (MEDA) based biochips are emerging microdroplets handling technology that empowers supervised fluids governance on a set of microelectrodes. The MEDA-based architecture enables the dynamic routing of droplets with variable sizes for better accuracy and convenience. Efficient droplet routing with prevention of cross-contamination and maintaining all fluidic restriction is the key challenging area on the MEDA-based biochips. We use a two-stage method that involves global and detailed routing. In order to determine the route capacity of every feasible routing path for each droplet, a graph denoting the capacity has been created during the global routing phase. The proposed method assigns the priority of each net depending on the influence factors of the other nets and blockages present in the bioassay. The proposed approach enables 80% of droplet routing without any cross-contamination, based on the First Priority Movement (FPM) and Second Priority Movement (SPM) in the first stage. A capacity graph provides maximum droplets flow using FPM and finds the suitable channel to reshape the size of the droplets to avoid collision on the routing paths to accomplish 100% routing. Experimental results demonstrate that even in complex bio-assays, our proposed phase-wise router reduces 20% of the latest arrival time (Tla) and minimizes 9% average time (Tavg) by decreasing 15% of microelectrodes count compared to other routing protocols. [ABSTRACT FROM AUTHOR]

The antibubble has emerged as a promising tool for the microdroplet manipulation since the intermediate air film can protect the inner globule from external contaminants. Moreover, the antibubble structure allows the convenient package and release of microdroplets since the intermediate air film would not hinder the separation between the inner globule and the liquid surface. Despite the development of various methods for antibubble formation, the initial approach involving single drop impact on a free liquid surface has received limited attention in subsequent studies, partly due to the challenges in replicating this phenomenon in practical applications. This paper presents an experimental investigation into antibubble formation via single drop impact on a liquid surface. Experimental results imply that antibubble formation requires the droplet to penetrate deeply into the liquid bath before the intermediate air film collapses or the deformed liquid surface contracts. A theoretical analysis is introduced to emphasize the crucial role of the density difference between the droplet and the liquid bath. A higher density of the droplet results in an increased penetration speed into the liquid bath, facilitating the formation of antibubbles. Notably, this study repeats the experimental results reported by Hughes and Hughes in 1932. Moreover, the method provides a means to control antibubble parameters such as diameter and air film thickness. This control offers valuable insight for subsequent investigations on antibubbles, establishing a foundation for further exploration and application of this intriguing phenomenon. [ABSTRACT FROM AUTHOR]

Microdroplets have been widely used in different fields due to their unique properties, such as compartmentalization, single-molecule sensitivity, chemical and biological compatibility, and high throughput. Compared to intricate and labor-intensive microfluidic techniques, the centrifuge-based method is more convenient and cost-effective for generating droplets. In this study, we developed a handy injection molding based method to readily produce monodisperse droplets by centrifugation. Briefly, we used two three-dimensional (3D) printed master molds with internal cavities to forge two coupled sub-molds by injecting polydimethylsiloxane (PDMS) and casted these two PDMS sub-molds into a nested structure that clamps the micro-channel array (MiCA) by injecting polyurethane resin. This method enables the generation of various sizes of monodispersed microdroplets by centrifugation with proper parameters within 10 min. To assess the performance of this method, homogeneous fluorescent hydrogel microspheres were generated and droplet digital polymerase chain reaction (ddPCR) was carried out. Overall, this method offers high-throughput droplet generation, reduces costs compared to other methods, and is user-friendly. [ABSTRACT FROM AUTHOR]

We report examples of C(sp2)−N, C(sp2)−S, and C(sp2)−P bond‐forming transformations in water microdroplets at room temperature and atmospheric pressure using N2 as a nebulizing gas. When an aqueous solution of vinylic acid and amine is electrosprayed (+3 kV), the corresponding C(sp2)−N product is formed in a single step, which was characterized using mass spectrometry (MS) and tandem mass spectrometry (MS2). The scope of this reaction was extended to other amines and other unsaturated acids, including acrylic (CH2=CHCOOH) and crotonic (CH3CH=CHCOOH) acids. We also found that thiols and phosphines are viable nucleophiles, and the corresponding C(sp2)−S and C(sp2)−P products are observed in positive ion mode using MS and MS2. [ABSTRACT FROM AUTHOR]