Opposite Charge Research Articles

Vortex molecules in a spin–orbit-coupled spin-1 condensate

A vortex molecule is predicted in a spin–orbit-coupled spin-1 Bose–Einstein condensate. This type of asymmetric soliton features four off-axis vortices and none of them coincide. There are two vortices of the same charge in the first and the third component, respectively, and two vortices of the opposite charge in the second component. This particular arrangement of vortices constitute a spin vortex molecule which is connected by a domain wall in the spin texture. In the dynamical simulation, we find the vortex molecule is static at the equilibrium but vibrates once it deviates from the equilibrium. The vibration mechanism is identified: fragmentation and coalescence. The vortex molecule exhibits mixing of ferromagnetic and antiferromagnetic states, where the meron-pair or bimeron is hidden. Our results suggest a way of creating bimeron-like vortex molecules in spin-1 Bose–Einstein condensates.

Ion permeability profiles of renal paracellular channel-forming claudins.

Members of the claudin protein family are the major constituents of tight junction strands and determine the permeability properties of the paracellular pathway. In the kidney, each nephron segment expresses a distinct subset of claudins that form either barriers against paracellular solute transport or charge- and size-selective paracellular channels. It was the aim of the present study to determine and compare the permeation properties of these renal paracellular ion channel-forming claudins. MDCK II cells, in which the five major claudins had been knocked out (claudin quintupleKO), were stably transfected with individual mouse Cldn2, -4, -8, -10a, -10b, or -15, or with dog Cldn16 or -19, or with a combination of mouse Cldn4 and Cldn8, or dog Cldn16 and Cldn19. Permeation properties were investigated in the Ussing chamber and claudin interactions by FRET assays. Claudin-4 and -19 formed barriers against solute permeation. However, at low pH values and in the absence of HCO3 -, claudin-4 conveyed a weak chloride and nitrate permeability. Claudin-8 needed claudin-4 for assembly into TJ strands and abolished this anion preference. Claudin-2, -10a, -10b, -15, -16+19 formed highly permeable channels with distinctive permeation profiles for different monovalent and divalent anions or cations, but barriers against the permeation of ions of opposite charge and of the paracellular tracer fluorescein. Paracellular ion permeabilities along the nephron are strictly determined by claudin expression patterns. Paracellular channel-forming claudins are specific for certain ions and thus lower transepithelial resistance, yet form barriers against the transport of other solutes.

Peptide-Based Complex Coacervates Stabilized by Cation-π Interactions for Cell Engineering.

Complex coacervation is a form of liquid-liquid phase separation, whereby two types of macromolecules, usually bearing opposite net charges, self-assemble into dense microdroplets driven by weak molecular interactions. Peptide-based coacervates have recently emerged as promising carriers to deliver large macromolecules (nucleic acids, proteins and complex thereof) inside cells. Thus, it is essential to understand their assembly/disassembly mechanisms at the molecular level in order to tune the thermodynamics of coacervates formation and the kinetics of cargo release upon entering the cell. In this study, we designed histidine-rich peptides consisting of modular sequences in which we systematically incorporate cationic, anionic, or aromatic residues at specific positions along the sequence in order to modulate intermolecular interactions and the resulting coacervation stability. We show that cation-π interactions between arginine and aromatic side chains are particularly efficient in stabilizing complex coacervates, and these interactions can be disrupted in the protein-rich intracellular environment, triggering the disassembly of complex coacervates followed by cargo release. With the additional grafting of a disulfide-based self-immolative side chain, these complex coacervates exhibited enhanced stability and could deliver proteins, mRNA, and CRISPR/Cas9 genome editing tools with tunable release kinetics into cells. This capability extends to challenging cell types, such as macrophages. Our study highlights the critical role of cation-π interactions in the design of peptide-based coacervates, expanding the biomedical and biotechnology potential of this emerging intracellular delivery platform.

Microstructure and Viscoelasticity of Oppositely Charged Ionomer Blend Melts

Microstructure and Viscoelasticity of Oppositely Charged Ionomer Blend Melts

Self-powered Wraparound (Abaxial) Droplet Deposition via a Superhydrophobic Surface Aid.

Many diseases and pests are fond of the backs of leaves, making wraparound deposition essential for enhancing agrochemical utilization and minimizing environmental hazards. We present a superhydrophobic surface decorated with fluorinated-SiO2 nanoparticles on the adaxial (front) side, improving sprayed droplet wraparound behaviors and achieving a 10-fold increase in abaxial (backside) deposition without using an electrostatic sprayer. Solid-liquid contact electrification boosts the positive charge-to-mass ratio of rebound spraying from 17 to 454 nC g-1, with the abaxial surface acquiring opposite electric charges at kilovolt-level voltages. This intensified droplet-solid electrostatic attraction guides droplets to wrap around and deposit on the abaxial surface. Further, a homemade fluorinated superhydrophobic tube enhances spray charge and abaxial deposition density on superhydrophobic plant leaves by 47- and 5- times, respectively, compared to those obtained via direct spraying. This work will significantly improve agrochemical efficiency, reducing environmental risks in sustainable agriculture and related industries.

Performance of Ti/TiO2-ZIF-67 photoanode under LED irradiation applied to the photoelectrodegradation of the antidepressant venlafaxine (VEN) in municipal wastewater effluent

This work describes the direct deposition of ZIF-67 metal-organic framework (MOF) onto Ti/TiO2 nanotubes forming a photoanode for the degradation of the antidepressant Venlafaxine (VEN). This material combines the excellent characteristics of ZIF-67 MOF in enhancing photocatalytic reduction and oxidation reactions induced by UV LED irradiation, as well as the storage of VEN molecules in its pores. Ti/TiO2-ZIF-67 features an eco-friendly technology for degradation of pharmaceutical micropollutants such as antidepressants. The photoanode was prepared, characterized and applied in the degradation of VEN by photocatalysis (PC), electrocatalysis (EC), photolysis (PL) and PEC processes. PEC process presented the best performance when compared to the others processes in both simulated solutions and real wastewater, achieving 100% and 89% degradation of VEN after 60 and 90 min, with TOC removal rates of 50% and 4%, respectively. The lower mineralization rate suggests that the degradation of VEN in complex matrices such as that of real wastewater produced recalcitrant by-products that are difficult to convert into CO2 and H2O. Zeta potential measurement showed that at pH 6 and 8 there is an effect of attraction of opposite electrostatic charges between the surface of ZIF-67 (positive) and VEN (negative), favoring the degradation of VEN in this pH range. The good performance of the Ti/TiO2-ZIF-67 can be attributed to the formation of the Z-scheme heterojunction between the TiO2 nanotubes and the ZIF-67 MOF which contributed to a lower rate of electron-hole (e-/h+) pairs recombination, favoring VEN degradation mainly to higher generation of •OH radical and less contribution of O2•- superoxide produced by UV irradiation forming some degradation by-products through demethylation and oxidation reactions.

Water-Soluble Iron Porphyrins as Catalysts for Suppressing Chlorinated Disinfection Byproducts in Hypochlorite-Dependent Water Remediation.

We are facing a world-wide shortage of clean drinking water which will only be further exacerbated by climate change. The development of reliable and affordable methods for water remediation is thus of utmost importance. Chlorine (which forms active hypochlorites in solution) is the most commonly used disinfectant due to its reliability and low cost. One drawback is that it reacts with organic pollutants to generate toxic chlorinated byproducts. To mitigate chlorination in water remediation, we have investigated the use of catalytic amounts of charged water-soluble iron porphyrins. These are known to activate hypochlorite to generate high valent oxoiron species. We studied the depletion of the model micropollutant phenol and the accumulation of chlorinated disinfection byproducts under water remediation conditions, using iron porphyrins [(TMPyP)FeCl]Cl4 and (NH4)4[(TPPS)FeCl] as catalysts, by membrane inlet mass spectrometry. Despite bearing opposite charges on the meso-substituent, both iron porphyrins suppress the formation of chlorinated disinfection by-products equally well. To gain further insight, spectroscopic studies were performed. These showed the transient formation of Compound II, followed by either regeneration of the iron(III) porphyrin at low NaOCl concentrations, or total decomposition of the porphyrin complex at high NaOCl concentrations. Potential future directions for modifications of porphyrin-based catalysts are discussed.

Polymer-immobilized 2D nonclose-packed colloidal crystals

Abstract We present a novel methodology for immobilizing 2D nonclose-packed colloidal crystals in polymer resins. In our previous work (Aoyama Y, Toyotama A, Okuzono T, Yamanaka J. Two-Dimensional Nonclose-Packed Colloidal Crystals by the Electrostatic Adsorption of Three-Dimensional Charged Colloidal Crystals. 2019. Langmuir 35, 9194.), we detailed a fabrication technique involving electrostatic adsorption of 3D charged colloidal crystals onto a glass substrate with an opposite charge. Drying is essential for producing durable materials as these structures are formed in an aqueous environment. However, merely drying the crystals can lead to considerable disruption of the particle arrangement because of the capillary forces that arise between the particles during water evaporation. In this study, we demonstrate the immobilization of 2D colloidal silica crystals in a polymer resin. First, we introduced a water-soluble polymer, poly(dimethyl acrylamide), which effectively adsorbs both the particles and the substrate to stabilize the crystals, followed by the evaporation of water. Various configurations of 2D colloidal silica crystals were successfully fixed onto the glass substrates. After immobilization with poly(dimethyl acrylamide), the dimethyl acrylamide monomer was added and underwent polymerization, resulting in a more robust entrapment of the colloidal crystals in the polymer resin. This method can be applied to other polymers and hydrophobic particles. The current findings are expected to be valuable for a broad range of photonic applications.

Mineralized Nanofiber Substrates Enabling High-Performance Dually Charged Nanofiltration Membranes with Enhanced Permeability.

Nanofiltration membranes (NFMs) with superior permeability and high rejection of both divalent anions and cations are highly desirable to meet the increasing separation demands of complex systems. Herein, we propose a three-in-one strategy to develop a state-of-the-art dually charged thin-film composite (TFC) nanofiltration membrane consisting of a positively charged electrospun nanofiber substrate (NFS) with surface mineralization and a negatively charged polyamide (PA) selective layer prepared by interfacial polymerization (IP). The highly hydrophilic mineralized nanofiber substrate not only effectively reduces the thickness of the PA selective layer but also crumples its structures by the abundant zirconia nanoparticles on the substrate surface, resulting in excellent water flux (15.0 L m-2 h-1 bar-1) for the TFC NFMs. The relationship between the thickness of the selective layer and substrate is further investigated using dissipative particle dynamics (DPD) simulations. Meanwhile, the dually charged NFM exhibits relatively high rejection for both anions (97.1% for Na2SO4 and 97.9% for MgSO4) and cations (87.9% for MgCl2) in aqueous solutions compared with single-charged membranes, which is attributed to the dual-repulsion effect of the selective layer and the substrate surface bearing opposite charges. Moreover, the prepared NFMs exhibit good stability and excellent antifouling performance. This work may pave the way for the development of highly efficient nanofiltration membranes for the practical separation of comprehensively charged solutes.

Modeling indirectly detected analyte peaks in ion-pair reversed-phase chromatography

In indirect detection, sample components lacking detectable properties are detected by adding a detectable component to the eluent, a so-called probe that interacts with the analytes to be detected. This study focuses on modeling indirect detection in two principally different cases. In case (1), the analyte component has the same charge as the probe component, so the probe acts as a co-ion of the analyte. In case (2), the analyte component has the opposite charge to the probe, so the probe acts as a counter-ion of the analyte.In the co-ion case (1), the analytes are alkyl sulfonates, and a competitive bi-Langmuir isotherm model was used. In the counter-ion case (2), the analytes are amines, and a modified bi-Langmuir isotherm model, incorporating ion-pairing on the stationary phase surface, was derived and applied for simulating the elution profiles. The chromatographic system comprised an XBridge Phenyl column as the stationary phase and an acetonitrile/phosphate buffer mixture with varying concentrations of sodium 2-naphthalenesulfonate as the eluent. In both cases, the detectable probe component was sodium 2-naphthalenesulfonate.The applied isotherm models successfully predicted system peaks with high agreement in both model cases, with calculated relative errors in retention times typically below 4.72 % and often below 1 %. The models were employed to predict the sensitivity of analytical methods, demonstrating excellent agreement between experimental and calculated sensitivities. These findings confirm the validity of the new adsorption isotherm model under these experimental conditions.

Ordered assemblies of peptide nanoparticles with only positive charge

Surface charge patchiness of different charge types can influence the solution behaviours of colloidal particles and globular proteins. Herein, coiled-coil ‘bundlemer’ nanoparticles that display only a single type of surface charge (SC) are computationally designed to compare their solution behaviours to mixed charge-type (MC) counterparts with both positively and negatively charged side chains. Nematic and columnar liquid crystal phases are discovered in low concentrations of SC particles, indicative of particle end-to-end stacking into columns combined with lateral electrostatic repulsion between columns, while MC particles with the same net charge and particle shape produced only amorphous, soluble aggregates. Similarly, porous lattices are formed in mixtures of SC/MC particles of opposite charges while MC/MC mixtures of opposite charges produce only amorphous aggregates. The lattice structure is inferred with a machine learning optimization approach. The differences between SC and MC particle behaviours directly show the importance of surface electrostatic patchiness.

Electrochemical Reactions Affected by Electric Double Layer Overlap in Conducting Nanopores.

When a potential is applied to an electrode immersed in an electrolyte solution, ions with opposite charges accumulate around the electrode, forming an electrical double layer (EDL). Unlike flat electrodes, nanoporous electrodes with pore sizes comparable to the EDL thickness experience overlapping EDLs, altering the electrochemically effective surface area. Although previous research has primarily examined the ion charging dynamics and EDL formation in nanoporous electrodes, the impact of EDL overlap on Faraday reactions remains underexplored. In this study, we examined the influence of EDL overlap on electrochemical reactions within nanoporous electrodes using chronoamperometry and DC and AC voltammetry. We used the electrolyte concentration, measurement duration, overpotential, and electrode material as variables to determine the relationship between the extent of EDL overlap and the electrochemical reaction. The electrolyte concentration-dependent electrochemical reaction due to the EDL overlap was more pronounced for electrodes with faster potential changes, shorter measurement times, lower overpotentials, and slower catalytic activity. This is a unique nanoporous electrochemical phenomenon that is not observed on flat electrodes. These findings provide insight into the utilization of nanoporous electrodes in catalytic and sensor applications.

U(1)-charged Dark Matter in three-Higgs-doublet models

We explore three-Higgs-doublet models that may accommodate scalar Dark Matter where the stability is based on an unbroken U(1)-based symmetry, rather than the familiar ℤ2 symmetry. Our aim is to classify all possible ways of embedding a U(1) symmetry in a three-Higgs-doublet model. The different possibilities are presented and compared. All these models contain mass-degenerate pairs of Dark Matter candidates due to a U(1) symmetry unbroken (conserved) by the vacuum. Most of these models preserve CP. In the CP-conserving case the pairs can be seen as one being even and the other being odd under CP or as having opposite charges under U(1). Not all symmetries presented here were identified before in the literature, which points to the fact that there are still many open questions in three-Higgs-doublet models. We also perform a numerical exploration of the U(1) × U(1)-symmetric 3HDM, this is the most general phase-invariant (real) three-Higgs-doublet model. The model contains a multi-component Dark Matter sector, with two independent mass scales. After imposing relevant experimental constraints we find that there are possible solutions throughout a broad Dark Matter mass range, 45–2000 GeV, the latter being a scan cutoff.

Driving Forces in the Formation of Biocondensates of Highly Charged Proteins: A Thermodynamic Analysis of the Binary Complex Formation.

A thermodynamic analysis of the binary complex formation of the highly positively charged linker histone H1 and the highly negatively charged chaperone prothymosin α (ProTα) is detailed. ProTα and H1 have large opposite net charges (-44 and +53, respectively) and form complexes at physiological salt concentrations with high affinities. The data obtained for the binary complex formation are analyzed by a thermodynamic model that is based on counterion condensation modulated by hydration effects. The analysis demonstrates that the release of the counterions mainly bound to ProTα is the main driving force, and effects related to water release play no role within the limits of error. A strongly negative Δcp (=-0.87 kJ/(K mol)) is found, which is due to the loss of conformational degrees of freedom.

Orthogonal Phase Transfer of Oppositely Charged FeII 4L6 Cages.

Coordination cages and their encapsulated cargo can be manoeuvred between immiscible liquid layers in a process referred to as phase transfer. Among the stimuli reported to drive phase transfer, counterion exchange is the most widespread. This method exploits the principle that counterions contribute strongly to the solubility preferences of coordination cages, and involves exchanging hydrophilic and hydrophobic counterions. Nevertheless, phase transfer of anionic cages remains relatively unexplored, as does selective phase transfer of individual cages from mixtures. Here we compare the phase transfer behaviour of two FeII 4L6 cages with the same size and geometry, but with opposite charges. As such, this study presents a rare example wherein an anionic cage undergoes phase transfer upon countercation exchange. We then combine these two cages, and demonstrate that their quantitative separation can be achieved by inducing selective phase transfer of either cage. These results represent unprecedented control over the movement of coordination cages between different physical compartments and are anticipated to inform the development of next-generation supramolecular systems.

On the similar spectral manifestations of protonic and hydridic hydrogen bonds despite their different origin

Previously studied complexes with protonic and hydridic hydrogen bonds exhibit significant similarities. The present study provides a detailed investigation of the structure, stabilization, electronic properties, and spectral characteristics of protonic and hydridic hydrogen bonds using low-temperature infrared (IR) spectroscopy and computational methods. Complexes of pentafluorobenzene with ammonia (C₆F₅H⋯NH₃) and triethylgermane with trifluoroiodomethane (Et₃GeH⋯ICF₃) were analyzed using both experimental and computational tools. Additionally, 30 complexes with protonic hydrogen bonds and 30 complexes with hydridic hydrogen bonds were studied computationally. Our findings reveal that, despite the opposite atomic charges on the hydrogens in these hydrogen bonds, and consequently the opposite directions of electron transfer in protonic and hydridic hydrogen bonds, their spectral manifestations - specifically, the red shifts in the X–H stretching frequency and the increase in intensity - are remarkably similar. The study also discusses the limitations of the current IUPAC definition of hydrogen bonding in covering both types of H-bonds and suggests a way to overcome these limitations.

Investigation of the synergistic effects of SiO2 and Al2O3 nanoparticles with SDS and CTAB surfactants on the stability and improving phase behavior of water-oil emulsions

The stability of emulsions is a significant challenge across various industries, including food, pharmaceutical, and petroleum. Surface-active agents utilized for enhanced oil recovery often exhibit inadequate performance under reservoir conditions with high salinity, presenting a critical barrier to effective emulsion stabilization. Furthermore, due to the extreme hydrophilic or hydrophobic nature of nanoparticles (NPs), they are not effective in stabilizing emulsions on their own. To address this limitation, a minimal quantity of surfactant was introduced into the NPs to improve their wettability and achieve dual wettability. This research has examined the synergistic effects of SiO₂ and Al₂O₃ NPs combined with sodium dodecyl sulfate (SDS) and cetyltrimethylammonium bromide (CTAB) surfactants on water-oil emulsion stability. This approach enhances emulsion stability by combining the stabilizing effects of both the NPs and the surfactants, an aspect that has not been previously addressed in phase behavior studies through the examination of the interactions and surface behavior of surfactant-nanoparticle complexes at the oil-water interface. Several experiments, including phase behavior, FT-IR, zeta potential, contact angle, and interfacial tension (IFT) tests, were performed to evaluate the interaction of surfactants with NPs. The results demonstrate that combining NPs with surfactants, especially those with opposite charges, significantly reduces IFT to the order of 10−6 mN/m, which can overcome capillary pressure, and enhances optimal salinity levels even up to 75000 ppm. Interactions between CTAB-SiO₂ and SDS-Al₂O₃ notably improve the hydrophobicity of NPs, resulting in IFT reductions of 11.4 and 7 mN/m, respectively, compared to NPs alone.

Tailor-Made Heterocharged Covalent Organic Framework Membrane for Efficient Ion Separation.

Pore size sieving, Donnan exclusion, and their combined effects seriously affect ion separation of membrane processes. However, traditional polymer-based membranes face some challenges in precisely controlling both charge distribution and pore size on the membrane surface, which hinders the ion separation performance, such as heavy metal ion removal. Herein, the heterocharged covalent organic framework (COF) membrane is reported by assembling two kinds of ionic COF nanosheets with opposite charges and different pore sizes. By manipulating the stacking quantity and sequence of two kinds of nanosheets, the impact of membrane surface charge and pore size on the separation performance of monovalent and multivalent ions is investigated. For the separation of anions, the effect of pore size sieving is dominant, while for the separation of cations, the effect of Donnan exclusion is dominant. The heterocharged TpEBr/TpPa-SO3H membrane with a positively charged upper layer and a negatively charged bottom layer exhibits excellent rejection of multivalent anions and cations (Ni2+, Cd2+, Cr2+, CrO4 2-, SeO3 2-, etc). The strategy provides not only high-performance COF membranes for ion separation but also an inspiration for the engineering of heterocharged membranes.

Effect of CO2 mixing on the rheological and electrochemical properties of fresh mortar at the early age

The study aimed to elucidate the mechanism behind rheological modification due to CO2 mixing at the mixing and post-mixing stages from an electrochemical perspective. The results indicated that CO2 mixing reduced the flowability while increasing penetration resistance and static yield stress. The electrostatic attraction between particles with opposite surface charges and the bridging effect of calcium carbonate constitute the primary factors for influencing the rheological properties of mortar at an early age. The altered surface charge of carbonized cement particles, primarily resulting from CO2 injection lowering the pH and ion concentration, reversed the zeta potential of particles from the traditionally negative charge (−3.59 mV) to a positive value (+13.3 mV). Furthermore, CO2 mixing further enhanced the dissolution of cement particles and accelerated the hydration process, thereby increasing the rate of structural build-up. CO2 mixing was demonstrated to be a potential rheological modifier for 3D-printed concrete applications.

Observation of quantum entanglement in top quark pair production in proton-proton collisions ats=13 TeV.

Entanglement is an intrinsic property of quantum mechanics and is predicted to be exhibited in the particles produced at the Large Hadron Collider. A measurement of the extent of entanglement in top quark-antiquark (tt¯) events produced in proton-proton collisions at a center-of-mass energy of 13 TeV is performed with the data recorded by the CMS experiment at the CERN LHC in 2016, and corresponding to an integrated luminosity of 36.3 fb-1. The events are selected based on the presence of two leptons with opposite charges and high transverse momentum. An entanglement-sensitive observableDis derived from the top quark spin-dependent parts of thett¯production density matrix and measured in the region of thett¯production threshold. Values ofD<-1/3are evidence of entanglement andDis observed (expected) to be-0.480-0.029+0.026(-0.467-0.029+0.026) at the parton level. With an observed significance of 5.1 standard deviations with respect to the non-entangled hypothesis, this provides observation of quantum mechanical entanglement withintt¯pairs in this phase space. This measurement provides a new probe of quantum mechanics at the highest energies ever produced.