Charged Beads Research Articles

PH-induced morphological reversible transition from microparticles to vesicles for effective bacteria entrapment

Polymer particles with stimuli-responsive properties offer promising applications in healthcare, chemical reactors, development of artificial cells and organelles, as well as in the entrapment of bacteria. In this study, a novel biocompatible, biodegradable, and pH-responsive diblock copolymer based on polylactide (PLA) and poly(2-(diisopropylamino)ethyl methacrylate) (PDPA) was synthesized via a metal-free one-pot/simultaneous ring-opening polymerization (ROP) and reversible addition-fragmentation chain transfer (RAFT) approach (ROP/RAFT). This copolymer was then employed to produce highly monodisperse microparticles using microfluidics droplet generation technique. Utilizing confocal microscopy imaging, a reversible pH-induced morphological transition from microparticles to vesicle-like structures was observed at pH 5.1. The reversible shift in morphology from microparticles to giant vesicles (Vs) in acidic environments is triggered by the protonation of amino groups of the PDPA block, rendering vesicle surfaces positively charged − an advantageous feature for attracting and engulfing negatively charged bacteria. Initial validation involved electrostatic interactions with negatively charged latex resin beads followed by assessing interaction capabilities with gram-negative bacteria, Escherichia coli (E. coli). Additionally, the reversible morphological transition of microparticles-to-vesicles was employed to study drug release at different pHs. This approach proven to be a promising strategy for targeted drug delivery and bacteria entrapment using smart pH-responsive microparticles.

Evaluation of a new beads reflux control microcatheter in drug-eluting bead transarterial chemoembolization

Rationale and objectivesA new microcatheter was recently developed claiming to reduce beads reflux in drug-eluting bead transarterial chemoembolization (DEB-TACE). The aim of this study was to compare the reflux control microcatheter ability versus a standard microcatheter for TACE treatment in patients with hepatocellular carcinoma. Material and methodsPatients were prospectively included between November 2017 and February 2022. They received a DEB-TACE treatment with charged radiopaque beads using standard microcatheters or the SeQure reflux control microcatheter (Guerbet, France) and were assigned respectively to a control and a test group. Beads distribution mismatch was evaluated between the targeted territory on treatment planning CBCT and beads’ spontaneous opacities on the post-intervention CBCT and the 1-month CT scanner. ResultsTwenty-three patients (21 men, median age 64 years [12.5 years]) with 37 hepatocellular carcinoma nodules were treated. The control group consisted of 13 patients – 19 nodules, while the test group included ten patients - 18 nodules. Non target embolization (NTE) was found in 20 % (2/10) of patients in the test group and 85 % (11/13) in the control group. NTE involved only an adjacent segment in the test group while it affected the adjacent biliary sector or even the contralateral liver lobe in the control group. No complication linked to NTE was found in the test group, while it led to one case of ischemic cholangitis and another case of biloma in the control group. ConclusionThe reflux control microcatheter may be efficient in reducing NTE and thus eventual adverse events in comparison to standard of care end-hole microcatheters.

A Structure Independent Molecular Fragment Interfuse Model for Mesoscale Dissipative Particle Dynamics Simulation of Peptides.

There is a need to develop robust computational models for mesoscale simulation of the structure of peptides over large length scales toward the discovery of novel peptides for medical applications to address the issues of peptide aggregation, enzymatic degradation, and short half-life. The primary objective was to predict the structure and conformation of peptides whose native structures are not known. This work presents a new model for computation of interaction parameters between the beads in coarse-grained dissipative particle dynamics (DPD) simulation that is properly calibrated for amino acids, supports compressibility requirement of water molecules, and accounts for subtle differences in the structure of amino acids and the charge in the side chain of charged amino acids. This new model is referred to as Structure Independent Molecular Fragment Interfuse Model, abbreviated as SIMFIM, because it accounts for specific interactions between different beads, which represent molecular fragments of the amino acids, in calculating nonbonded interaction parameters in the absence of knowing the actual peptide structure. The electrostatic interactions are incorporated in this model by using a normal distribution of charges around the center of the beads to prevent the collapse of oppositely charged soft beads. The uniquely parameterized DPD force field in the SIMFIM model is optimized for a given peptide with respect to the degree of coarse-grained graining for simulating the peptide over long times and length scales. The SIMFIM model was tested in this work using four peptides, namely, TrpZip2, Rubrivinodin, Lihuanodin, and IC3-CB1/Gai peptides, whose structures were sourced from the Protein Data Bank. The SIMFIM model predicted radius of gyration (Rg) values for the peptides closer to the actual structures as compared to the conventional model, and there was less deviation between the predicted and actual structures of the peptides.

Constant-pH Simulations of a Coarse-Grained Model of Polyfunctional Weak Charged Biopolymers

A coarse-grained model of linear polyfunctional weak charged biopolymers was implemented, formed of different proportions of acid-base groups resembling the composition of humic substances. These substances are mainly present in dissolved organic matter in natural water. The influence of electrostatic interactions computing methods, factors concerning the structure of the chain, different functional groups, and the ionic strength on polyelectrolytes were studied. Langevin dynamics with constant pH simulations were performed using the ESPResSO package and the Python-based Molecule Builder for ESPResSo (pyMBE) library. The coverage was fitted to a polyfunctional Frumkin isotherm, with a mean-field interaction between charged beads. The composition of the chain affects the charge while ionic strength affects both the charge and the radius of gyration. Additionally, the parameters intrinsic to the polyelectrolyte model were well reproduced by fitting the polyfunctional Frumkin isotherm. In contrast, the non-intrinsic parameters depended on the ionic strength. The method developed and applied to a polyfunctional polypeptide model, that resembles a humic acid, will be very useful for characterizing biopolymers with several acid-base functional groups, where their structure, the composition of the different functional groups, and the determination of the main intrinsic proton binding constants and their proportion are not exactly known.

PH-induced morphological transition of aggregates formed by miktoarm star polymers in dilute solution: a mesoscopic simulation study.

The self-assembly of miktoarm star polymers μ-A i (B(D)) j C k in a neutral solution and the pH-responsive behaviors of vesicles and spherical micelles in an acidic solution have been investigated by DPD simulation. The results show that the self-assembled morphologies can be regulated by the lengths of pH-responsive arm B and hydrophilic arm C, leading to the formation of vesicles, discoidal micelles, and spherical micelles in a neutral solution. The dynamic evolution pathways of vesicles and spherical micelles are categorized into three stages: nucleation, coalescence, and growth. Subsequently, the pH-responsive behaviors of vesicles and spherical micelles have been explored by tuning the protonation degree of pH-responsive arm B. The vesicles evolves from nanodisks to nanosheets, then to nanoribbons, as the protonation degree increases, corresponding to a decrease in pH value, while the spherical micelles undergoes a transition into worm-like micelles, nanosheets, and nanoribbons. Notably, the electrostatic interaction leads the counterions to form a regular hexagonal pattern in nanosheets, while an alternative distribution of charged beads has been observed in nanoribbons. Furthermore, the role of the electrostatic interaction in the morphological transition has been elucidated through the analysis of the distribution of positive and negative charges, as well as the electrostatic potential for associates.

Assessment of the MARTINI 3 Performance for Short Peptide Self-Assembly.

The coarse-grained MARTINI force field, initially developed for membranes, has proven to be an exceptional tool for investigating supramolecular peptide assemblies. Over the years, the force field underwent refinements to enhance accuracy, enabling, for example, the reproduction of protein-ligand interactions and constant pH behavior. However, these protein-focused improvements seem to have compromised its ability to model short peptide self-assembly. In this study, we assess the performance of MARTINI 3 in reproducing peptide self-assembly using the well-established diphenylalanine (FF) as our test case. Unlike its success in version 2.1, FF does not even exhibit aggregation in version 3. By systematically exploring parameters for the aromatic side chains and charged backbone beads, we established a parameter set that effectively reproduces tube formation. Remarkably, these parameter adjustments also replicate the self-assembly of other di- and tripeptides and coassemblies. Furthermore, our analysis uncovers pivotal insights for enhancing the performance of MARTINI in modeling short peptide self-assembly. Specifically, we identify issues stemming from overestimated hydrophilicity arising from charged termini and disruptions in π-stacking interactions due to insufficient planarity in aromatic groups and a discrepancy in intermolecular distances between this and backbone-backbone interactions. This investigation demonstrates that strategic modifications can harness the advancements offered by MARTINI 3 for the realm of short peptide self-assembly.

Bacteriophage Engineering for Improved Copper Ion Binding.

In this study, fd viruses are genetically modified to display seven cropped versions (H, HG, HGF, HGFA, HGFAN, HGFANV and HGFANVA) of the previously identified Cu(II) specific peptide (HGFANVA). Atomic force microscopy (AFM) imaging reveals the typical filamentous structures of recombinant phages with thicknesses of ≈2-5nm in dry state. Scanning electron microscopy (SEM) imaging shows that HGFANVA viruses form larger elongated assemblies than H viruses that are deposited with a mineral layer after Cu(II) treatment. C and N peaks are detected for virus samples through Energy dispersive X-ray spectroscopy (EDX) analyses confirming the presence of phage organic material. Cu peak is only detected for engineered viruses after Cu(II) exposure. Enzyme-linked immunosorbent assay (ELISA) analyses show the selective Cu(II) binding of engineered phages. Agarose gel electrophoresis (AGE) and zeta potential analyses reveal negative surface charges of engineered viral constructs. Positively charged Cytopore beads are coated with bacteriophages and used for Cu(II) ion sorption studies. ICP-MS analyses clearly show the improved Cu(II) binding of engineered viruses with respect to wild-type fd phages. Such bottom-up constructed, genetically engineered virus-based biomaterials may be applied in bioremediation studies targeting metal species from environmental samples.

Explosomes: A new modality for DEB-TACE local delivery of sorafenib: In vivo proof of sustained release

The current medical practice in treating Hepatocellular carcinoma (HCC) using Drug Eluting Transarterial chemoembolization (DEB-TACE) technique is limited only to hydrophilic ionizable drugs, that can be attached ionically to the oppositely charged beads. This limitation has forced physicians to subscribe the more hydrophobic, first treatment option drugs, like sorafenib systemically via the oral route, thus flooding the patient system with a very powerful, non-specific, multiple-receptor tyrosine kinase inhibitor that is associated with notorious side effects. In this paper, a new modality is introduced, where highly charged, drug loaded liposomes are added to oppositely charged DEBs in a manner causing them to “explode” and the drug is eventually attached to the beads in the lipid patches covering their surfaces; therefore we call them “Explosomes”. After fully describing the preparation process and in vitro characterization, this manuscript delves into an in vivo pharmacokinetic study over 50 New Zealand rabbits, where explosomal loading is challenged vs oral as well as current practice of emulsifying sorafenib in lipiodol. Over 14 days of follow up, and compared to other groups, explosomal loading of SRF on embolic beads proved to cause a slower release pattern with longer Tmax, lower Cmax and less washout to general circulation in healthy animals. This treatment modality opens a new untapped door for local sustained delivery of hydrophobic drugs in catheterized organs.

Molecular Crowders Can Induce Collapse in Hydrophilic Polymers via Soft Attractive Interactions.

A comprehensive understanding of protein folding and biomolecular self-assembly in the intracellular environment requires obtaining a microscopic view of the crowding effects. The classical view of crowding explains biomolecular collapse in such an environment in terms of the entropic solvent excluded volume effects subjected to hard-core repulsions exerted by the inert crowders, neglecting their soft chemical interactions. In this study, the effects of nonspecific, soft interactions of molecular crowders in regulating the conformational equilibrium of hydrophilic (charged) polymers are examined. Using advanced molecular dynamics simulations, collapse free energies of an uncharged, a negatively charged, and a charge-neutral 32-mer generic polymer are computed. The strength of the polymer-crowder dispersion energy is modulated to examine its effect on polymer collapse. The results show that the crowders preferentially adsorb and drive the collapse of all three polymers. The uncharged polymer collapse is opposed by the change in solute-solvent interaction energy but is overcompensated by the favorable change in the solute-solvent entropy as observed in hydrophobic collapse. However, the negatively charged polymer collapses with a favorable change in solute-solvent interaction energy due to reduction in the dehydration energy penalty as the crowders partition to the polymer interface and shield the charged beads. The collapse of a charge-neutral polymer is opposed by the solute-solvent interaction energy but is overcompensated by the solute-solvent entropy change. However, for the strongly interacting crowders, the overall energetic penalty decreases since the crowders interact with polymer beads via cohesive bridging attractions to induce polymer collapse. These bridging attractions are found to be sensitive to the binding sites of the polymer, since they are absent in the negatively charged or uncharged polymers. These interesting differences in thermodynamic driving forces highlight the crucial role of the chemical nature of the macromolecule as well as of the crowder in determining the conformational equilibria in a crowded milieu. The results emphasize that the chemical interactions of the crowders should be explicitly considered to account for the crowding effects. The findings have implications in understanding the crowding effects on the protein free energy landscapes.

On-line dual-stage enrichment via magneto-extraction and electrokinetic preconcentration: A new concept and instrumentation for capillary electrophoresis

This study reports on the development of a new concept of on-line dual preconcentration stages for capillary electrophoresis (CE), in which two completely different preconcentration approaches can be realized in the same capillary. In the first stage, a dynamic magneto-extraction of target analytes on circulating magnetic beads is implemented within the capillary. In the second one, electrokinetic preconcentration of eluted analytes via large volume sample stacking is carried out to focus them into a nano band, prior to CE separation of enriched analytes. To implement the dual-stage preconcentration operation, a purpose-made instrument was designed, combining electrophoretic and microfluidic modules to allow precise control of the movement of magnetic beads and analyte's flow. The potential of this new enrichment principle and its associated instrument was demonstrated for CE separation with light-emitting-diode-induced fluorescent (LEDIF) detection of target double-stranded DNA (ds-DNA). The workflow consists of purification and preconcentration of a target DNA fragment (300 bp) on negatively charged magnetic beads, followed by in-capillary elution and fluorescent labelling of the enriched DNA. Large volume sample stacking of the DNA eluent was then triggered to further preconcentrate the labelled DNA before its analysis by CE-LEDIF. An enrichment factor of 125 was achieved for the target DNA fragment. With our new approach, dual-stage sample pretreatment and CE separation can now be performed in-capillary without any mismatch of working volumes, nor any waste of pretreated samples.

Salt-Induced Transformations of Hybrid Micelles Formed by Anionic Surfactant and Poly(4-vinylpyridine).

Salt-induced structural transformation of charged hybrid surfactant/polymer micelles formed by potassium oleate and poly(4-vinylpyridine) was investigated by cryo-TEM, SANS with contrast variation, DLS, and 2D NOESY. Cryo-TEM data show, that at small salt concentration beads-on-string aggregates on polymer chains are formed. KCl induces the transformation of those aggregates into rods, which is due to the screening of the electrostatic repulsion between similarly charged beads by added salt. In a certain range of salt concentration, the beads-on-string aggregates coexist with the rodlike ones. In the presence of polymer, the sphere-to-rod transition occurs at higher salt concentration than in pure surfactant system indicating that hydrophobic polymer favors the spherical packing of potassium oleate molecules. The size of micelles was estimated by DLS. The rods that are formed in the hybrid system are much shorter than those in polymer-free surfactant solution suggesting the stabilization of the semi-spherical endcaps of the rods by embedded polymer. 2D NOESY data evidence that in the spherical aggregates the polymer penetrates deep into the core, whereas in tighter packed rodlike aggregates it is located mainly at core/corona interface. According to SANS with contrast variation, inside the rodlike aggregates the polymer adopts more compact coil conformation than in the beads-on-string aggregates. Such adaptive self-assembled polymer-surfactant nanoparticles with water-insoluble polymer are very promising for various applications including drag reduction at transportation of fluids.

TEMPO-oxidized cellulose beads for cationic dye adsorption

Toxic organic dyes present in wastewater should be removed before discharge. In this study, TEMPO-oxidized, regenerated cellulose beads were prepared using a simple falling ball technique for cationic methylene blue (MB) removal. The obtained cellulose beads were characterized using various analytical techniques. The results indicated that TEMPO-oxidized cellulose beads displayed porous structures with high content of carboxylic acid groups. Thus, the negatively charged cellulose beads can effectively adsorb cationic MB with an adsorption capacity of 495 mg/g at a starting concentration of 100 mg/L. This simple one-step adsorption process achieved near-complete MB removal at pH 7, indicating strong electrostatic interactions between cationic MB and negatively charged oxidized cellulose beads. The experimental data can be well described by the Langmuir isotherm model and the Pseudo-second-order model. The fabricated cellulose beads exhibit great potential for practical application in dye removal from wastewater.

Phase Diagram Study of Catanionic Surfactants Using Dissipative Particle Dynamics.

Dissipative particle dynamics (DPD) simulations has been performed to study the phase transition of a mixture of cationic and anionic surfactants in an aqueous solution as a function of the total concentration in water and the relative ratio of surfactants. The impact of the relative difference between the tail lengths of the cationic and anionic surfactants on the phase diagram has been simulated by tuning the number of DPD beads in the simulation model. This research also discusses the impact of the frequently used values of the parameters associated with the harmonic bonds among the bonded DPD beads on the obtained self-assemblies. We find remarkable differences in the resultant self-assemblies based on different choices of harmonic bond parameters. The performed simulations show an enhanced spectrum of self-assemblies with augmented tail lengths and disparate harmonic bond parameters. The obtained self-assemblies are quite unique and can potentially be used in the future for various applications. We also compare the simulation results of the vesicle structures obtained by modeling the electrostatic interaction in the simulation among the charged beads by explicitly introducing charges with a long-range interaction with those obtained by tuning the implicit electrostatic interaction without the long-range interaction. The effects of the chain length of the model and the harmonic bond parameters on the internal density of DPD beads and stress profiles within the vesicles are examined closely. These results are a significant contribution to understanding the stability of the phases and tailoring of the desired vesicles.

Development of a microfluidic droplet platform with an antibody-free magnetic-bead-based strategy for high through-put and efficient EVs isolation

In this study, we present a novel microfluidic droplet-based strategy for high performance isolation of extracellular vesicles (EVs). For EVs capture and release, a magnetic bead-based approach without having recourse to any antibody was optimized in batch and then adapted to the microfluidic droplet system. This antibody-free capture approach relies on the presence of a water-excluding polymer, polyethylene glycol (PEG), to precipitate EVs on the surface of negatively charged magnetic beads. We significantly improved the reproducibility of EV recovery and avoided positive false bias by including a washing step and optimizing the protocol. Well-characterized EV standards derived from pre-purified bovine milk were used for EVs isolation performance evaluation. An EVs recovery of up to 25% estimated with nanoparticle tracking analysis (NTA) was achieved for this batchwise PEG-based approach. The confirmation of isolated EVs identity was also made with our recently developed method using capillary electrophoresis (CE) coupled with laser-induced fluorescent (LIF) detection. In parallel, a purpose-made droplet platform working with magnetic tweezers was developed for translation of this PEG-based method into a droplet microfluidic protocol to further improve the performance in terms of EVs capture efficiency and high throughput. The droplet-based protocol offers a significant improvement of recovery rate (up to 50%) while reducing sample and reagent volumes (by more than 10 folds) and operation time (by 3 folds) compared to the batch-wise mode.

Trench-shaped field-effect transistor integrates electronic particle detection with microfluidics

Silicon design simultaneously detects electrical and optical signals from charged fluorescent beads.

Trench field-effect transistors integrated in a microfluidic channel and design considerations for charge detection.

Field-effect transistors (FETs) combined with a microfluidic system allow for the electrical detection of charged materials moving in a microfluidic channel. Here, we demonstrate trench-shaped silicon FETs with the combination of a microfluidic channel that can be used for simultaneous electrical and optical detection of charged fluorescent beads. The n-channel silicon trench FETs have a maximum transconductance of 1.83 × 10-5 S at near-zero gate bias voltage, which is beneficial for the high sensitivity of electrical detection. The optical transparency and physical robustness of the integrated microfluidic channel are achieved by a polydimethylsiloxane (PDMS)/glass hybrid cover combining the good sealing characteristics of PDMS, and the thin and flat properties of glass. Device evaluation methodologies and measurement approaches are also presented demonstrating a synchronized time-lapse imaging and electronic detection of bead transport. The proposed device and design consideration could advance the promise of electronic sensing to measure potential differences induced by charged analytes.

Important Role of Concave Surfaces in Deposition of Colloids under Favorable Conditions as Revealed by Microscale Visualization.

This study conducted saturated column experiments to systematically investigate deposition of 1 μm positively charged polystyrene latex micro-colloids (representing microplastic particles) on negatively charged rough sand, glass beads, and soil with pore water velocities (PWV) from 4.9 × 10-5 to 8.8 × 10-4 m/s. A critical value of PWV was found below which colloidal attachment efficiency (AE) increased with increasing PWV. The increase in AE with PWV was attributed to enhanced delivery of the colloids and subsequent attachment at concave locations of rough collector surfaces. The AE decreased with further increasing PWV beyond the threshold because the convex sites became unavailable for colloid attachment. By simulating the rough surfaces using the Weierstrass-Mandelbrot equation, the extended Derjaguin-Landau-Verwey-Overbeek (XDLVO) interaction energy calculations and torque analysis revealed that the adhesive torques could be reduced to be comparable or smaller than hydrodynamic torques even under the favorable conditions. Interestingly, scanning electron microscopic experiments showed that blocking occurred at convex sites at all ionic strengths (ISs) (e.g., even when the colloid-colloid interaction was attractive), whereas at concave sites, blocking and ripening (i.e., attached colloids favor subsequent attachment) occurred at low and high ISs, respectively. To our knowledge, our work was the first to show coexistence of blocking and ripening at high ISs due to variation of the collector surface morphology.

Observation of Red Blood Cell Membrane Charge Using Magnetic Beads Under Pulsed Magnetic Field

Aggregation of red blood cells (RBC) is one of many factors that impair vascular circulation and is closely related to the zeta potential. Pulsed magnetic field (PMF) is effective in improving RBC aggregation and mobility. Therefore, this study aims to observe indirectly the change of RBC membrane charges using negatively charged magnetic beads (MBs) and to elucidate the effect of PMF on RBC aggregation via zeta potential. Since concentrations of hematocrit (Ht) and plasma are different for each person, in order to objectify the zeta potential, RBC suspension was prepared using phosphate buffered saline (PBS) which is a protein-free buffer and prevents RBC agglomerating. Tert-butyl hydroperoxide (tBHP) was also used to oxidize agents to understand RBC aggregation in an environment of tumor cells or inflammation. Our PMF stimulator has a maximum intensity of 0.27 T at a transition time of <inline-formula xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink"> <tex-math notation="LaTeX">$102 \mu \text{s}$ </tex-math></inline-formula> with pulse intervals of 1 Hz. The number of RBCs attached to MB was higher in the PMF group than in the control group. In addition, in the oxidized blood, the number of RBCs attached to MB decreased compared to that of the control group, but it was increased after PMF treatment. In the PMF-treated group, a larger number of MBs attached to RBCs was also observed. Our results could be interpreted that the instantaneous flux change of PMF increases negative charge density on RBC membrane, thereby increasing zeta potential between RBCs, inducing disaggregation of RBCs, thus eventually contributing to the improvement of blood circulation. PMF suggests the possibility of being used as a noninvasive treatment for preventing blood circulation disorder. Further study needs to verify the effect of PMF on the changes in plasma concentration in patients with cardiovascular diseases such as atherosclerosis, thrombosis, and hypertension.

Electrostatic Interaction-Based Fabrication of Calcium Alginate-Zein Core-Shell Microcapsules of Regulable Shapes and Sizes.

Core-shell microcapsules with combined features of hydrophilicity and hydrophobicity have become much popular. However, the assembly of biocompatible and edible materials in hydrophilic-hydrophobic core-shell microcapsules is not easy. In this work, based on electrostatic interactions, we prepared controllable calcium alginate (ALG)-zein core-shell particles of different shapes and sizes using hydrophilic ALG and hydrophobic zein by a two-step extrusion method. Negatively charged hydrogel beads of spherical, ellipsoidal, or fibrous shape were added into a positively charged zein solution (dissolved in 70% (v/v) aqueous ethanol solution) to achieve different-shaped core-shell particles. Interestingly, the size, shape, and shell thickness of the particles can be regulated by the needle diameter, stirring speed, and zein concentration. Moreover, for simplification, the core-shell particles were also synthesized by a one-step extrusion method, in which an ALG solution was added dropwise into a 70% (v/v) aqueous ethanol solution containing zein and CaCl2. The particles synthesized in this work showed controlled digestion of encapsulated medium-chain triglyceride (MCT) and sustained release of encapsulated thiamine and ethyl maltol. Our preparation method is simplistic and can be extended to fabricate a variety of hydrophilic and hydrophobic core-shell structures to encapsulate a broad spectrum of materials.

Dielectric Coatings for Resistive Pulse Sensing Using Solid-State Pores.

The present study reports on the systematic characterization of the effectiveness of dielectric coating to tailor capture-to-translocation dynamics of single particles in solid-state pores. We covered the surface of SiNx membranes with SiO2, HfO2, Al2O3, TiO2, or ZnO, which allowed us to change the ζ-potential at the pore wall, reflecting the isoelectric points of these coating materials. Resistive pulse measurements of negatively charged polystyrene beads elucidated more facile electrophoretic capture of the particles and slower translocation motions in the channel under more negative electric potential at the oxide surface. These findings provide a guide to engineer pore wall surface for optimizing the translocation dynamics for efficient sensing of particles and molecules.