Long-range Electrostatic Forces Research Articles

The Interaction and Lift-Off Forces of an Atomic Force Microscope Tip from Single Fibers Extracted from Protective Clothing Fabric.

The widespread use of engineered nanoparticles (ENPs) poses a potential health hazard to humans, especially to those involved in either nanoparticle manufacturing or the usage and assembly of a final product. In this study, we performed systematic force vs distance experiments (F(z)) using an atomic force microscope (AFM) on fibers commonly used in street clothing and protective laboratory clothing to better characterize the relevant interaction forces between engineered nanoparticles (ENPs) and the contacted fabric fibers. The intent of this study is to identify those factors that influence the interaction of ENPs with fabrics with an aim to improve the efficacy of protective clothing against ENP exposure and mitigate potential health risks. A ∼14 nm diameter AFM SiOx tip (with nanoscale radius of curvature) is considered as an effective oxide ENP. Features present (or absent) in a well-executed F(z) AFM experiment provide a fingerprint that distinguishes the relevant forces and interaction mechanisms in play. Measurements of F(z) as a function of relative humidity were also performed to assess the importance of thin surface water layers in binding nanometer-size oxide ENPs to a fabric fiber. The F(z) data indicate the dominant mechanism for adhesion of the oxide tip to the various fabric fibers (cotton, Tyvek (HD polyethylene), polypropylene, and polyester) can be attributed to a van der Waals interaction. The analysis provides no evidence for long-range electrostatic forces or capillary-induced adhesion of the AFM tip to the fibers studied.

Long-range electrostatic forces in periodic structures: The development of adjustable wave filters

In this work, we examine the effects of electrostatic forces on wave propagation in periodic structures. The research explores how these structures, a type of metamaterial, can have their vibrational characteristics altered by interactions that are non-local. In this work, it is demonstrated how electrostatic forces influence dispersion curves and the resultant metamaterial properties. These findings have implications for developing tunable metamaterials, with potential applications in various fields, such as tunable wave-beaming devices and filters. This research contributes to a deeper understanding of the complex interactions in metamaterials and their practical applications.

Characterization of LL37 Binding to Collagen through Peptide Modification with a Collagen-Binding Domain.

Collagen-based biomaterials loaded with antimicrobial peptides (AMPs) present a promising approach for promoting wound healing while providing protection against infections. In our previous work, we modified the AMP LL37 by incorporating a collagen-binding domain (cCBD) as an anchoring unit for collagen-based wound dressings. We demonstrated that cCBD-modified LL37 (cCBD-LL37) exhibited improved retention on collagen after washing with PBS. However, the binding mechanism of cCBD-LL37 to collagen remained to be elucidated. In this study, we found that cCBD-LL37 showed a slightly higher affinity for collagen compared to LL37. Our results indicated that cCBD inhibited cCBD-LL37 binding to collagen but did not fully eliminate the binding. This suggests that cCBD-LL37 binding to collagen may involve more than just one-site-specific binding through the collagen-binding domain, with non-specific interactions also playing a role. Electrostatic studies revealed that both LL37 and cCBD-LL37 interact with collagen via long-range electrostatic forces, initiating low-affinity binding that transitions to close-range or hydrophobic interactions. Circular dichroism analysis showed that cCBD-LL37 exhibited enhanced structural stability compared to LL37 under varying ionic strengths and pH conditions, implying potential improvements in antimicrobial activity. Moreover, we demonstrated that the release of LL37 and cCBD-LL37 into the surrounding medium was influenced by the electrostatic environment, but cCBD could enhance the retention of peptide on collagen scaffolds. Collectively, these results provide important insights into cCBD-modified AMP-binding mechanisms and suggest that the addition of cCBD may enhance peptide structural stability and retention under varying electrostatic conditions.

Accelerated Hybridization Chain Reaction Kinetics Using Poly DNA Tetrahedrons and Its Application in Detection of Aflatoxin B1.

Traditional hybridization chain reaction (HCR) as a popular isothermal amplification technique shows some inevitable disadvantages in bioanalysis due to its relatively slow kinetics, which could be markedly promoted when the HCR initiator occurs under tension. Herein, a poly DNA tetrahedrons (pTDNs)-mediated HCR was successfully constructed to make its initiator in a stretched state by long-range electrostatic forces owing to the superimposed electrostatic interactions derived from the synthesized pTDNs, and it was hypothesized that it could remarkably enhance HCR performance, which was testified by theoretical simulations and experimental studies. Consequently, pTDNs-mediated HCR was applied to develop a novel immunoassay for rapid and sensitive detection of aflatoxin B1 as a proof-of-concept, and its signal amplification was attributed to the increased G4 DNAzyme that loaded on the second antibody. Our work paves a promising way using simple DNA frameworks alone to heighten HCR kinetics for reaction speed improvement and signal amplification in bioanalysis.

Conformal order and Poincaré-Klein mapping underlying electrostatics-driven inhomogeneity in tethered membranes.

Understanding the organization of matter under the long-range electrostatic force is a fundamental problem in multiple fields. In this work, based on the electrically charged tethered membrane model, we reveal regular structures underlying the lowest-energy states of inhomogeneously stretched planar lattices by a combination of numerical simulation and analytical geometric analysis. Specifically we show the conformal order characterized by the preserved bond angle in the lattice deformation and reveal the Poincaré-Klein mapping underlying the electrostatics-driven inhomogeneity. The discovery of the Poincaré-Klein mapping, which connects the Poincaré disk and the Klein disk for the hyperbolic plane, implies the connection of long-range electrostatic force and hyperbolic geometry. We also discuss lattices with patterned charges of opposite signs for modulating in-plane inhomogeneity and even creating 3D shapes, which may have a connection to metamaterials design. This work suggests the geometric analysis as a promising approach for elucidating the organization of matter under the long-range force.

Electrostatic interactions control the adsorption of extracellular vesicles onto supported lipid bilayers

Communication between cells located in different parts of an organism is often mediated by membrane-enveloped nanoparticles, such as extracellular vesicles (EVs). EV binding and cell uptake mechanisms depend on the heterogeneous composition of the EV membrane. From a colloidal perspective, the EV membrane interacts with other biological interfaces via both specific and non-specific interactions, where the latter include long-ranged electrostatic and van der Waals forces, and short-ranged repulsive “steric-hydration” forces. While electrostatic forces are generally exploited in most EV immobilization protocols, the roles played by various colloidal forces in controlling EV adsorption on surfaces have not yet been thoroughly addressed. In the present work, we study the adsorption of EVs onto supported lipid bilayers (SLBs) carrying different surface charge densities using a combination of quartz crystal microbalance with dissipation monitoring (QCM-D) and confocal laser scanning microscopy (CLSM). We demonstrate that EV adsorption onto lipid membranes can be controlled by varying the strength of electrostatic forces and we theoretically describe the observed phenomena within the framework of nonlinear Poisson-Boltzmann theory. Our modelling results confirm the experimental observations and highlight the crucial role played by attractive electrostatics in EV adsorption onto lipid membranes. They furthermore show that simplified theories developed for model lipid systems can be successfully applied to the study of their biological analogues and provide new fundamental insights into EV-membrane interactions with potential use in developing novel EV separation and immobilization strategies.

Electrospun heterojunction nanofibrous membranes for photoinduced enhancement of fine particulate matter capture in harsh environment

Particulate matter (PM) pollution has posed a severe threat to the environment and human health. Especially for submicron-level fine particulate PM0.3, it is still difficult to achieve high-efficiency filtration. Herein, we loaded TiO2/g-C3N4 (TCN) heterojunction photocatalyst on polystyrene/polyacrylonitrile (PS/PAN) multiscale nanofiber membranes by a simple one-step blending electrospinning technique. Due to the strong long-range electrostatic force of the built-in electric field, the composite membrane has a remarkably enhanced filtration effect under light. Even under harsh conditions with a high PM0.3 concentration of more than 1,800,000 m−3 and a high flow rate of 25 L/min, it still has a high filtration efficiency of greater than 98.5%, an increase of about 20% compared with dark conditions, and the pressure drop is only low to 94 Pa. More importantly, the electrostatic field can be regenerated with light, and this preparation strategy can be effectively extended to other photocatalyst heterojunctions.

On the Chemical Potential of Many-Body Perturbation Theory in Extended Systems.

Finite-temperature many-body perturbation theory in the grand-canonical ensemble is fundamental to numerous methods for computing electronic properties at nonzero temperature, such as finite-temperature coupled-cluster. In most applications it is the average number of electrons that is known rather than the chemical potential. Expensive correlation calculations must be repeated iteratively in search for the interacting chemical potential that yields the desired average number of electrons. In extended systems with mobile charges the situation is particular, however. Long-ranged electrostatic forces drive the charges such that the average ratio of negative and positive charges is one for any finite chemical potential. All properties per electron are expected to be virtually independent of the chemical potential, as they are in an electric wire at different voltage potentials. This work shows that per electron, the exchange-correlation free energy and the exchange-correlation grand potential indeed agree in the infinite-size limit. Thus, only one expensive correlation calculation suffices for each system size, sparing the search for the interacting chemical potential. This work also demonstrates the importance of regularizing the Coulomb interaction such that each electron on average interacts only with as many electrons as there are electrons in the simulation, avoiding interactions with periodic images. Numerical calculations of the warm uniform electron gas have been conducted with the Spencer-Alavi regularization employing the finite-temperature Hartree approximation for the self-consistent field and linearized finite-temperature direct-ring coupled-cluster doubles for treating correlation.

Insight on bulk shear strength parameters of clay using discrete element approach incorporating physics-based interparticle force model

This paper aims to provide insight on factors affecting the bulk shear strength parameters of clay, i.e., the cohesion and internal friction as well as the effects of memory of preconsolidation pressure. A unique Discrete Element Method (DEM) model is built on platy particles with customized particle interaction force model. The particle interaction force model considers non-contact forces (such as the long-range electrostatic repulsion, short-range van der Waals attraction) as well as the direct contact force. The long-range electrostatic forces are calibrated by measurement with Atomic Force Microscope (AFM). Parameters for direct particle contacts of the regular DEM contact model, such as the contact stiffness and the friction coefficient, are calibrated by use of experimental consolidation and direct shear testing data. Computational simulations are conducted on digital clay specimen subjected to virtual direct shear tests. The predicted experimental responses of the digital specimens are consistent with typically observed in experiments including the shear stress-shear strain relationship, volumetric contraction and dilation, shear band formation, etc. From the stress–strain curves, the soil strength parameters are obtained with common experimental criteria. The DEM simulation results show that higher preconsolidation pressure drives more particles to overcome non-contact force into direct contacts and consequently bonding by van der Waals force. Consequently, the bulk cohesion of clay increases with increasing preconsolidation pressure. The results show that bulk cohesion strength is mainly attributed to the attractive interparticle force as well as the interlocking of platy particle, while the bulk internal friction angle is affected by the particle friction coefficient and particle fabric. Overall, the simulation results indicate the experimentally observed macroscopic shear strength parameters c and φ are linked to the microscope characteristics of soil particles and their mutual interactions. The results offer insight on the microscopic properties of particles on the bulk macroscopic strength behaviors. Besides, this work demonstrates a new strategy for simulation-based prediction of bulk soil strength parameters, by incorporating microscale characterization of the interparticle interactions and particle fabric into the particle-based DEM model.

Theory of Layered-Oxide Cathode Degradation in Li-ion Batteries by Oxidation-Induced Cation Disorder

Disorder-driven degradation phenomena, such as structural phase transformations and surface reconstructions, can significantly reduce the lifetime of Li-ion batteries, especially those with nickel-rich layered-oxide cathodes. We develop a general free energy model for layered-oxide ion-intercalation materials as a function of the degree of disorder, which represents the density of defects in the host crystal. The model accounts for defect core energies, long-range dipolar electrostatic forces, and configurational entropy of the solid solution. In the case of nickel-rich oxides, we hypothesize that nickel with a high concentration of defects is driven into the bulk by electrostatic forces as oxidation reactions at the solid-electrolyte interface reduce nickel and either evolve oxygen or oxidize the organic electrolyte at high potentials (>4.4 V vs Li/Li+). The model is used in battery cycling simulations to describe the extent of cathode degradation when using different voltage cutoffs, in agreement with experimental observations that lower-voltage cycling can substantially reduce cathode degradation. The theory provides a framework to guide the development of cathode compositions, coatings and electrolytes to enhance rate capability and enhance battery lifetime. The general theory of cation-disorder formation may also find applications in electrochemical water treatment and ion separations, such as lithium extraction from brines, based on competitive ion intercalation in battery materials.

Effect of electrostatic interaction on impact breakage of agglomerates formed by charged dielectric particles.

In this paper, the prototypical process of the normal impact of dense agglomerates is investigated using the discrete element method-boundary element method coupled simulations. The agglomerate consists of 50 charged particles with the surface energy equal to 10mJ/m^{2}. The particles are assumed to be tribocharged and follow an exponential charge distribution, while the varying levels of coupled polarization are also considered. Simulation results reveal that the presence of the electrostatic interactions due to particle charging and polarization could drive more pronounced re-agglomeration after the collision, which effectively reduces the degree of agglomerate fragmentation. Moreover, when quantifying the collision outcomes using the fragmentation ratio, the influence of the electrostatic force is most significant at a moderate incident velocity. This is because, at such incident velocities, the impact is violent enough to break the agglomerate, but many ejected fragments are usually at low velocities and are attracted back by the long-range electrostatic force. Furthermore, the electrostatic force between same-sign particles even becomes attractive when particles are strongly polarized, leading to qualitative changes in particle dynamics. Finally, by comparing the collision outcomes under different incident velocities, the contact interactions are found to prevail when particles are still bounded in the agglomerate, while the electrostatic interaction becomes dominant after particles detach from each other.

Review of Electrostatic Force Calculation Methods and Their Acceleration in Molecular Dynamics Packages Using Graphics Processors.

Molecular dynamics (MD) simulations probe the conformational repertoire of macromolecular systems using Newtonian dynamic equations. The time scales of MD simulations allow the exploration of biologically relevant phenomena and can elucidate spatial and temporal properties of the building blocks of life, such as deoxyribonucleic acid (DNA) and protein, across microsecond (μs) time scales using femtosecond (fs) time steps. A principal bottleneck toward extending MD calculations to larger time scales is the long-range electrostatic force measuring component of the naive nonbonded force computation algorithm, which scales with a complexity of (N, number of atoms). In this review, we present various methods to determine electrostatic interactions in often-used open-source MD packages as well as the implementation details that facilitate acceleration of the electrostatic interaction calculation.

Silver-nanowire/bamboo-charcoal composite percolation network on nylon sheet for improved PM2.5 capture efficiency

Particulate matter (PM) pollution is a significant threat to the environment and public health, necessitating the development of efficient, easy-to-use, versatile protection and treatment devices. Herein, we rationally design a novel reusable composite filter for the high-efficiency capture of indoor fine PM with a particle diameter of <2 µm (PM2.5). The use of such filters is important for ensuring safe indoor environments. This study elucidates the manufacturing of filters based on electrostatic and adsorption principles using a silver-nanowire/bamboo-charcoal composite material to enhance PM elimination. The filter comprised silver nanowires with an 8 mg/mL concentration and bamboo charcoal with a 0.1% w/v concentration, dipped in nylon sheet for nine cycles and annealed at 120 °C for 15 min; the filter exhibited a minimum sheet resistance of 4.1 Ω/sq. Silver-nanowire/bamboo-charcoal composite percolation network filters use strong long-range electrostatic forces and adsorption to capture PM2.5, work in an active mode, and exhibit high efficiency (>99.9%), low power consumption, and reusability after simple washing. The proposed PM filter can be applied in environmental applications.

Dehydration-Rehydration Studies on Polytypes of Chloride and Nitrate Layered Double Hydroxides of Nordstrandite and Bayerite: a Comparative Study.

In this work, we report for the first time, the dehydration-rehydration studies of nordstrandite-derived layered double hydroxides (LDHs) of Li and Al, n-[Li–Al–X] (X = Cl– and NO3–) (n-nordstrandite derived). n-[Li–Al–NO3], an orthorhombic phase, dehydrated at 180 °C to a monoclinic phase. Refinement placed the NO3– ions parallel to the hydroxide layers. The dehydration showed no change in basal spacing. The monoclinic n-[Li–Al–Cl] dehydrated at 160 °C with a 0.49 Å compression in basal spacing to an orthorhombic polytype. We compared our results with the published results of their bayerite counterparts b-[Li–Al-X] (b-bayerite derived) and observed that though n-[Li–Al–X] and b-[Li–Al–X] LDHs have similar structures, their dehydrated phases are structurally different. We also report the refinement of b-[Li–Al–Cl] (DH). Previous studies attribute the basal spacing values to the (i) degree of hydration and (ii) orientation of anions in the interlayer. We observe that basal spacing is a manifestation of the symmetry of the crystal. Dehydration of nitrate intercalated LDH, which proceeds from an orthorhombic symmetry to a monoclinic symmetry with no decrease in the interlayer spacing, is attributed to sliding of the hydroxyl layers in the ab-plane due to the increase in the β value. This sliding stabilizes the interlayer through weak long-range electrostatic forces that mainly contribute to the stabilization of the layered structure at separations much larger than the effective radius of hydrogen bonds. Such stabilization would negate the need for the layers to compress, thus conserving the basal spacing in n-[Li–Al–NO3] (DH).

Oxygen vacancy assisted condensation of DNA molecule observed on ZnO thin film

An exotic condensation of DNA molecules is observed on the nanostructured ZnO surface. The ZnO nanostructures (NS) fabricated by thermal vapor deposition technique were associated with a large number of oxygen vacancies on the surface. These oxygen vacancies induced changes in the DNA conformation which further reflected through changes in the persistence length of the DNA molecules. This indicates a reinforcement of the bonds and binding in both the phosphate and the base regions of the DNA molecules with the positively charged core vacancy sites on the ZnO nanostructured surface through strong interaction mediated via long-range electrostatic forces which effectively reduced the end-to-end distance of the λ-DNA molecule. This strongly suggests a transition of the λ-DNA molecule through structural modification into a more compact higher-order fractal dimension from its native state.

(Invited) Crystal Phase Engineering of Cesium Lead Iodide By Nanoconfinement

Nanoscale dimensional reduction leads to perturbed electronic structure, a foundational concept in the study of quantum dots. In this work, we extend this concept to consider how nanoscale dimensionality perturbs the crystal phase diagram of a solid. We apply this to the phase behavior of cesium lead iodide, a material that possesses favorable optoelectronic properties in its perovskite crystal polymorph at high temperature, and exhibits an undesirable crystal phase at room temperature. We develop and test the hypothesis that for solids such as cesium lead iodide that simultaneously exhibit both predominantly covalent bonding (Pb—I) and predominantly ionic bonding (Cs—I), low-density, high-symmetry phases can be favored by restricting crystal dimensions below 100 nm. This is based on a model in which short-range, orbital-orbital repulsive forces, which favor low-density and high-symmetry phases, are in competition with long-range electrostatic forces, which favor high-density. The electrostatic forces, being long-range in nature, are more diminished by truncating the crystal. Experimentally, we show that the phase sequence can be inverted and the equilibrium shifted by as much as 250 ºC through various nanostructuring approaches, including colloidal nanocrystal co-assembly and crystallization within nanoporous scaffolds. Ultimately, we seek to develop a phase diagram in which temperature and size are the independent variables.

Long-range interactions in model colloidal dispersions with surface charge distributions

The theoretical model, which is based on the density functional approach, has been developed for studying the electrostatic properties of colloidal dispersions (modified colloidal primitive model; MCPM) containing hard-spherical ions with a homogeneous surface charge distribution. The mean-spherical approximation for the multi-component charged ions has been used to account for the electrostatic ion correlation effects. The present study reflects the importance of the charge distribution of macroion in determining the ionic structure and mean forces acting on the macroions. Compared with the MCPM, the colloidal primitive model (CPM), on which the colloidal charge is assumed to be in the center of particle, shows very long-range electrostatic properties and mean force acting on the macroions because of the strong cross correlation between the hard-sphere contribution and the Coulomb interaction. The long-range attractions and repulsions in the charged colloidal dispersions originate from the entropic effects and are found at high packing fractions of the colloidal ions.

Electrostatic attraction caused by triboelectrification in climbing geckos

Adhesion achieved through feet setae is fundamental for gecko agilely maneuvering. Although diverse hypotheses have been proposed, none of them thoroughly explains the setae function, implying a kind of hybrid-mechanism-based adhesion in geckos. In addition to van der Waals interactions and capillary force, the electrostatic attraction that emerges from triboelectrification was suggested as a component of setae adhesion. Nevertheless, the contribution by electrostatic attraction to the total setae attachment is still controversial. In this study, we analyzed the occurrence of electrostatic attraction at gecko setae through experiments and model analyses. By touching the substrates with only ∼1/70th of the foot area, freely wall-climbing geckos developed tribocharge at their feet setae with a density of ∼277 pC/mm2, generating electrostatic attractions with a strength of ∼4.4 mN/mm2. From this perspective, the adhesion driven by triboelectrification could account for about 1% of total adhesion. Model analyses at spatula level indicated a similar result showing that the electrostatic force might account for ∼3% of the adhesion that facilitates wall-climbing in geckos. The low contribution of the electrostatic force partly explains why geckos always face difficulty in maneuvering onto those substrates (e.g., teflon) where they could easily develop tribocharge but difficultly generate van der Waals force. However, long-range electrostatic forces may play other roles in a distance range where the van der Waals interaction cannot function. These findings not only add to our understanding of the mechanism of gecko adhesion, but also will help us advance gecko-inspired fibular adhesives.

The Role of Dimer Formation in the Nucleation of Superlattice Transformations and Its Impact on Disorder.

The formation of defect-free two-dimensional nanocrystal (NC) superstructures remains a challenge as persistent defects hinder charge delocalization and related device performance. Understanding defect formation is an important step toward developing strategies to mitigate their formation. However, specific mechanisms of defect formation are difficult to determine, as superlattice phase transformations that occur during fabrication are quite complex and there are a variety of factors influencing the disorder in the final structure. Here, we use Molecular Dynamics (MD) and electron microscopy in concert to investigate the nucleation of the epitaxial attachment of lead chalcogenide (PbX, where X = S, Se) NC assemblies. We use an updated implementation of an existing reactive force field in an MD framework to investigate how initial orientational (mis)alignment of the constituent building blocks impacts the final structure of the epitaxially connected superlattice. This Simple Molecular Reactive Force Field (SMRFF) captures both short-range covalent forces and long-range electrostatic forces and allows us to follow orientational and translational changes of NCs during superlattice transformation. Our simulations reveal how robust the oriented attachment is with regard to the initial configuration of the NCs, measuring its sensitivity to both in-plane and out-of-plane misorientation. We show that oriented attachment nucleates through the initial formation of dimers, which corroborate experimentally observed structures. We present high-resolution structural analysis of dimers at early stages of the superlattice transformation and rationalize their contribution to the formation of defects in the final superlattice. Collectively, the simulations and experiments presented in this paper provide insights into the nucleation of NC oriented attachment, the impact of the initial configuration of NCs on the structural fidelity of the final epitaxially connected superlattice, and the propensity to form commonly observed defects, such as missing bridges and atomic misalignment in the superlattice due to the formation of dimers. We present potential strategies to mitigate the formation of superlattice defects.

Multilevel polarization-fields enhanced capture and photocatalytic conversion of particulate matter over flexible schottky-junction nanofiber membranes

Atmospheric Particulate matter (PM) with small sizes has caused a serious air-pollution problem calling for high-performance PM-capture materials and promising remediation strategies. In this contribution, we propose a new idea to proactively capture PM and simultaneously in-situ convert the captured PM pollution over the flexible schottky-junctions nanofiber membrane (NFM) consisting of rutile TiO2 nanoparticles (NPs)-decorated electrospun carbon NFs. We also demonstrate that both the interfacial electron-transfer process at the TiO2/carbon schottky-junctions and the photo-excitation process at the surface of TiO2 NPs can induce polarization fields in the TiO2/carbon NFM due to the difference of the space-charge distribution. These multilevel polarization fields can drive the long-range electrostatic force to enhance the proactive PM-capture ability of the NFM. As such, the TiO2/carbon NFM exhibited a satisfactory quality factor (0.11 Pa−1) for balancing the PM2.5-filtration efficiency (99.92 %) and the pressure drop (only 63 Pa). More importantly, upon UV–vis-light irradiation, 92.98 % of the ultrafine PM0.3 was removed over this TiO2/carbon NFM. Furthermore, the as-captured PM on the NFM could be photocatalytically decomposed by the photoactive-component of TiO2 NPs, during which some of the carbonaceous PM was converted into the fuels of such CO and CH4 through a multi-step photoreaction.