Osmotic Forces Research Articles

Photocatalytic Magnetic Microgyroscopes with Activity-Tunable Precessional Dynamics.

Magnetic nano/microrotors are passive elements spinning around an axis due to an external rotating field while remaining confined to a plane. They have been used to date in different applications related to fluid mixing, drug delivery, or biomedicine. Here we realize an active version of a magnetic microgyroscope which is simultaneously driven by a photoactivated catalytic reaction and a rotating magnetic field. We investigate the uplift dynamics of this colloidal spinner when it precesses around its long axis while self-propelling due to the light induced decomposition of hydrogen peroxide in water. By combining experiments with theory, we show that activity emerging from the cooperative action of phoretic and osmotic forces effectively increases the gravitational torque, which counteracts the magnetic and viscous ones, and carefully measure its contribution. Finally, we demonstrate that by modulating the field amplitude, one can induce hysteresis loops in the uplift dynamics of the spinners.

The Role of the Swollen State in Cell Proliferation.

Cell swelling is known to be involved in various stages of the growth of plant cells and microorganisms but in mammalian cells how crucial a swollen state is for determining the fate of the cellular proliferation remains unclear. Recent evidence has increased our understanding of how the loss of the cell surface interactions with the extracellular matrix at early mitosis decreases the membrane tension triggering curvature changes in the plasma membrane and the activation of the sodium/hydrogen (Na +/H +) exchanger (NHE1) that drives osmotic swelling. Such a swollen state is temporary, but it is critical to alter essential membrane biophysical parameters that are required to activate Ca2 + channels and modulate the opening of K + channels involved in setting the membrane potential. A decreased membrane potential across the mitotic cell membrane enhances the clustering of Ras proteins involved in the Ca2 + and cytoskeleton-driven events that lead to cell rounding. Changes in the external mechanical and osmotic forces also have an impact on the lipid composition of the plasma membrane during mitosis.

Accumulation of Cerebrospinal Fluid, Ventricular Enlargement, and Cerebral Folate Metabolic Errors Unify a Diverse Group of Neuropsychiatric Conditions Affecting Adult Neocortical Functions.

Cerebrospinal fluid (CSF) is a fluid critical to brain development, function, and health. It is actively secreted by the choroid plexus, and it emanates from brain tissue due to osmolar exchange and the constant contribution of brain metabolism and astroglial fluid output to interstitial fluid into the ventricles of the brain. CSF acts as a growth medium for the developing cerebral cortex and a source of nutrients and signalling throughout life. Together with perivascular glymphatic and interstitial fluid movement through the brain and into CSF, it also acts to remove toxins and maintain metabolic balance. In this study, we focused on cerebral folate status, measuring CSF concentrations of folate receptor alpha (FOLR1); aldehyde dehydrogenase 1L1, also known as 10-formyl tetrahydrofolate dehydrogenase (ALDH1L1 and FDH); and total folate. These demonstrate the transport of folate from blood across the blood-CSF barrier and into CSF (FOLR1 + folate), and the transport of folate through the primary FDH pathway from CSF into brain FDH + ve astrocytes. Based on our hypothesis that CSF flow, drainage issues, or osmotic forces, resulting in fluid accumulation, would have an associated cerebral folate imbalance, we investigated folate status in CSF from neurological conditions that have a severity association with enlarged ventricles. We found that all the conditions we examined had a folate imbalance, but these folate imbalances were not all the same. Given that folate is essential for key cellular processes, including DNA/RNA synthesis, methylation, nitric oxide, and neurotransmitter synthesis, we conclude that ageing or some form of trauma in life can lead to CSF accumulation and ventricular enlargement and result in a specific folate imbalance/deficiency associated with the specific neurological condition. We believe that addressing cerebral folate imbalance may therefore alleviate many of the underlying deficits and symptoms in these conditions.

A Passive Perspiration Inspired Wearable Platform for Continuous Glucose Monitoring.

The demand for glucose monitoring devices has witnessed continuous growth from the rising diabetic population. The traditional approach of blood glucose (BG) sensor strip testing generates only intermittent glucose readings. Interstitial fluid-based devices measure glucose dynamically, but their sensing approaches remain either minimally invasive or prone to skin irritation. Here, a sweat glucose monitoring system is presented, which completely operates under rest with no sweat stimulation and can generate real-time BG dynamics. Osmotically driven hydrogels, capillary action with paper microfluidics, and self-powered enzymatic biochemical sensor are used for simultaneous sweat extraction, transport, and glucose monitoring, respectively. The osmotic forces facilitate greater flux inflow and minimize sweat rate fluctuations compared to natural perspiration-based sampling. The epidermal platform is tested on fingertip and forearm under varying physiological conditions. Personalized calibration models are developed and validated to obtain real-time BG information from sweat. The estimated BG concentration showed a good correlation with measured BG concentration, with all values lying in the A+B region of consensus error grid (MARD = 10.56% (fingertip) and 13.17% (forearm)). Overall, the successful execution of such osmotically driven continuous BG monitoring system from passive sweat can be a useful addition to the next-generation continuous sweat glucose monitors.

β-barrel proteins dictate the effect of core oligosaccharide composition on outer membrane mechanics.

The outer membrane is the defining cellular structure of Gram-negative bacteria, a group that contains many important pathogens like Escherichia coli , Vibrio cholerae , and Pseudomonas aeruginosa . One role of the outer membrane is to block the uptake of small molecules like antibiotics. However, it is becoming increasingly clear that it also functions as a structural exoskeleton that is critical for the cell's ability to cope with internal and external mechanical forces. Here, we carefully dissect the molecular basis for the load-bearing capacity of the outer membrane by screening a set of mutants with a new cell biophysics assay.

Crosslinking and Swelling Properties of pH-Responsive Poly(Ethylene Glycol)/Poly(Acrylic Acid) Interpenetrating Polymer Network Hydrogels.

This study investigates the crosslinking dynamics and swelling properties of pH-responsive poly(ethylene glycol) (PEG)/poly(acrylic acid) (PAA) interpenetrating polymer network (IPN) hydrogels. These hydrogels feature denser crosslinked networks compared to PEG single network (SN) hydrogels. Fabrication involved a two-step UV curing process: First, forming PEG-SN hydrogels using poly(ethylene glycol) diacrylate (PEGDA) through UV-induced free radical polymerization and crosslinking reactions, then immersing them in PAA solutions with two different molar ratios of acrylic acid (AA) monomer and poly(ethylene glycol) dimethacrylate (PEGDMA) crosslinker. A subsequent UV curing step created PAA networks within the pre-fabricated PEG hydrogels. The incorporation of AA with ionizable functional groups imparted pH sensitivity to the hydrogels, allowing the swelling ratio to respond to environmental pH changes. Rheological analysis showed that PEG/PAA IPN hydrogels had a higher storage modulus (G') than PEG-SN hydrogels, with PEG/PAA-IPN5 exhibiting the highest modulus. Thermal analysis via thermogravimetric analysis (TGA) and differential scanning calorimetry (DSC) indicated increased thermal stability for PEG/PAA-IPN5 compared to PEG/PAA-IPN1, due to higher crosslinking density from increased PEGDMA content. Consistent with the storage modulus trend, PEG/PAA-IPN hydrogels demonstrated superior mechanical properties compared to PEG-SN hydrogels. The tighter network structure led to reduced water uptake and a higher gel modulus in swollen IPN hydrogels, attributed to the increased density of active network strands. Below the pKa (4.3) of acrylic acid, hydrogen bonds between PEG and PAA chains caused the IPN hydrogels to contract. Above the pKa, ionization of PAA chains induced electrostatic repulsion and osmotic forces, increasing water absorption. Adjusting the crosslinking density of the PAA network enabled fine-tuning of the IPN hydrogels' properties, allowing comprehensive comparison of single network and IPN characteristics.

Colloidal Stability of PFSA-Ionomer Dispersions. Part I. Single-Ion Electrostatic Interaction Potential Energies.

Charged colloidal particles neutralized by a single counterion are increasingly important for many emerging technologies. Attention here is paid specifically to hydrogen fuel cells and water electrolyzers whose catalyst layers are manufactured from a perfluorinated sulfonic acid polymer (PFSA) suspended in aqueous/alcohol solutions. Partially dissolved PFSA aggregates, known collectively as ionomers, are stabilized by the electrostatic repulsion of overlapping diffuse double layers consisting of only protons dissociated from the suspended polymer. We denote such double layers containing no added electrolyte as "single ion". Size-distribution predictions build upon interparticle interaction potential energies from the Derjaguin-Landau-Verwey-Overbeek (DLVO) formalism. However, when only a single counterion is present in solution, classical DLVO electrostatic potential energies no longer apply. Accordingly, here a new formulation is proposed to describe how single-counterion diffuse double layers interact in colloidal suspensions. Part II (Srivastav, H.; Weber, A. Z.; Radke, C. J. Langmuir 2024 DOI: 10.1021/acs.langmuir.3c03904) of this contribution uses the new single-ion interaction energies to predict aggregated size distributions and the resulting solution pH of PFSA in mixtures of n-propanol and water. A single-counterion diffuse layer cannot reach an electrically neutral concentration far from a charged particle. Consequently, nowhere in the dispersion is the solvent neutral, and the diffuse layer emanating from one particle always experiences the presence of other particles (or walls). Thus, in addition to an intervening interparticle repulsive force, a backside osmotic force is always present. With this new construction, we establish that single-ion repulsive pair interaction energies are much larger than those of classical DLVO electrostatic potentials. The proposed single-ion electrostatic pair potential governs dramatic new dispersion behavior, including dispersions that are stable at a low volume fraction but unstable at a high volume fraction and finite volume-fraction dispersions that are unstable with fine particles but stable with coarse particles. The proposed single-counterion electrostatic pair potential provides a general expression for predicting colloidal behavior for any charged particle dispersion in ionizing solvents with no added electrolyte.

L version of the transformed Kedem-Katchalsky equations for membrane transport of electrolyte solutions and internal energy conversion.

One of the important formalisms of non-equilibrium thermodynamics is Peusner network thermodynamics. The description of the energy conversion in membrane processes, i.e., the conversion of the internal energy of the system into the dissipated energy and the free energy used for the work associated with the transport of solution components, allows us to describe the relationship between these energies and the thermodynamic forces acting in the membrane system. The aim of this study was to develop a procedure to transform the Kedem-Katchalsky equations for the transport of binary electrolytic solutions across a membrane into the Kedem-Katchalsky-Peusner equations based on Peusner network thermodynamics. The conversion of electrochemical energy to free energy in the membrane system was also determined. The nanobiocellulose biomembranes (Biofill) were the subject of the study with experimentally determined transport parameters for aqueous NaCl solutions. The research method is the Kedem-Katchalsky-Peusner formalism for binary electrolyte solutions with introduced Peusner coefficients. The coefficients of the L version of the membrane transport equations and the Peusner coupling coefficients were derived as functions of NaCl concentration in the membrane. Based on these coefficients, the fluxes of internal energy of the system, energy dissipated to the surroundings and free energy related to the transport of electrolyte across the membrane were calculated and presented as functions of the osmotic and electric forces on the membrane. The Peusner coefficients obtained from the transformations of the coefficients of the Kedem-Katchalsky formalism for the transport of electrolyte solutions through the Biofill membrane were used to calculate the coupling coefficients of the membrane processes and the dissipative energy flux. The dissipative energy flux takes the form of a quadratic form due to the thermodynamic forces on the membrane - second degree curves are obtained. Moreover, the dissipative energy flux as a function of thermodynamic forces allowed us to examine the energy conversion in transport processes in the membrane system.

Coupled instability modes at a solvent/non-solvent interface to decorate cellulose acetate flowers

Dispensing a water drop on the thin film of a solution composed of cellulose acetate (CA) in dimethyl formamide (DMF) forms a thin and porous CA layer at the water–DMF interface. While a denser water drop on a rarer CA–DMF film manifests a Rayleigh–Taylor instability—RTI, the dynamically forming porous layer at the water–DMF interface triggers a Saffman–Taylor instability—STI. The combined effects of RTI and STI enable the formation, growth, coalescence, and branching of an array of periodic finger patterns to finally develop into a flower-like morphology. A general linear stability analysis (GLSA) of a thin bilayer composed of a Newtonian and incompressible water layer resting on a Darcy–Brinkman porous medium could predict the length and the time scales of such a finger formation phenomenon. The GLSA uncovers the crucial roles of pressure gradients originating from the gravitational effects, osmotic forces, the Marangoni effect, and capillary forces on the dynamics of the finger formation. While the density difference between water and CA–DMF layer plays a crucial role in deciding the initial finger spacing, the osmotic pressure dictates the formation, growth, branching, and coalescence of fingers. The length-FL and number-Navg of fingers are found to scale as FL∼We0.33Re−0.25 and Navg∼We0.33Re0.25. Further, an inverse relationship of the concentration of CA (C) with ∼We−0.3 and ∼Re−0.7 highlights its role in the formation and growth of fingers. The loading of CA in DMF, the viscosity and density of the CA–DMF film, and the curvature of the fingers are found to be other parameters that decide morphologies.

ON THE INFLUENCE OF NON-EQUILIBRIUM VACANCIES ON THE CHARACTERISTICS OF STRAIN INDUCED BROKEN DISLOCATION BOUNDARIES

The influence of material supersaturation with deformation vacancies on the characteristics of broken dislocation boundaries that appear near wedge disclinations as a result of accommodative plastic deformation is considered. An analysis is made for the elastic and osmotic forces acting on the dislocations of the broken boundary. Using discrete dislocation dynamics method, computer simulation of the nonconservative motion (climb) of dislocations in the boundary plane has been carried out. The broken boundary formed as a result of the splitting of the original disclination into two partial with equal strengths and the boundary with an inhomogeneous distribution of dislocations (with a linearly decreasing misorientation) were considered as initial ones. It is shown that in the case of broken dislocation boundary formed near a positive wedge disclination, dislocation climb leads to its unlimited growth through the model grain with a simultaneous decrease of misorientation. In the case of a boundary formed near a negative disclination, the osmotic forces acting on the dislocations of the broken boundary can, at sufficiently large super saturations of the material with nonequilibrium vacancies, lead to its significant compression with a simultaneous increase of the density of the Burgers vector. In this case, the choice of the initial configuration of the broken boundary has practically no effect on the characteristics of the equilibrium distribution of dislocations. The density distributions of the Burgers vector along the broken boundary are calculated for the case of small and large supersaturations of the material with nonequilibrium vacancies. The critical value of supersaturation above which the boundary compression occurs is calculated. The boundary compression leads to a significant increase in tensile stresses in its vicinity. In this case, the maximum tensile stresses in the plane coinciding with the plane of the boundary are reached at the boundary break point. The results obtained may be of interest in the analysis of possible mechanisms for the initiation of cracks and pores during ductile fracture of metals.

Mathematical Model of Freezing of Rocks Saturated With Salt Solution Taking Into Account the Influence of Osmosis

The paper presents a mathematical model of rocks freezing saturated with salt solution under impact of osmotic force. Osmosis is related to the salt concentration gradient, which is characteristic for solutions, and it is a powerful mechanism for the movement of solutions in poorly permeable porous media. A mathematical criterion for the formation of closed “pockets” with brines (cryopags) in frozen rocks has been obtained. This criterion is shown to be significantly depends on the osmosis coefficient. The model includes three layers of a porous medium saturated, respectively, with ice, ice and solution, and salt solution only. A special case was studied when there is only a second layer with a movable boundary, on which a phase transition from the second layer to the third one occurs. The investigated layer is saturated with a salt solution and ice in thermodynamic equilibrium. Other layers are replaced by boundary conditions. An approximate analytical solution of the problem is found in a self-similar formulation. The nature of the influence of osmotic force on the freezing process of rocks saturated with solution is shown. The characteristic patterns associated with the considered process are revealed. One of the features of the osmosis influence is the fact that it can cause the movement (migration) of the solution in the direction of increasing pressure, i.e. in the direction opposite to the driving force caused by the pressure gradient.

Effect of mechanical stresses on viral capsid disruption during droplet formation and drying

Identification of the mechanisms by which viruses lose activity during droplet formation and drying is of great importance to understanding the spread of infectious diseases by virus-containing respiratory droplets and to developing thermally stable spray dried live or inactivated viral vaccines. In this study, we exposed suspensions of baculovirus, an enveloped virus, to isolated mechanical stresses similar to those experienced during respiratory droplet formation and spray drying: fluid shear forces, osmotic pressure forces, and surface tension forces at interfaces. DNA released from mechanically stressed virions was measured by SYBR Gold staining to quantify viral capsid disruption. Theoretical estimates of the force exerted by fluid shear, osmotic pressures and interfacial tension forces during respiratory droplet formation and spray drying suggest that osmotic and interfacial stresses have greater potential to mechanically destabilize viral capsids than forces associated with shear stresses. Experimental results confirmed that rapid changes in osmotic pressure, such as those associated with drying of virus-containing droplets, caused significant viral capsid disruption, whereas the effect of fluid shear forces was negligible. Surface tension forces were sufficient to provoke DNA release from virions adsorbed at air-water interfaces, but the extent of this disruption was limited by the time required for virions to diffuse to interfaces. These results demonstrate the effect of isolated mechanical stresses on virus particles during droplet formation and drying.

Upregulation of hypothalamic TRPV4 via S100a4/AMPKα signaling pathway promotes the development of diet-induced obesity

Obesity is associated with abnormal regulation of energy metabolism in the hypothalamus. Transient receptor potential vanilloid 4 (TRPV4) is involved in regulating osmotic pressure, temperature and mechanical force transmission, but little is known about its role in obesity. Herein, the present study aimed to elucidate the effect of hypothalamic TRPV4 on high-fat diet-induced obesity (DIO) and evaluate its potential for regulating energy metabolism. Here we show that hypothalamic TRPV4 content is increased in DIO rats. Central administration of adeno-associated virus expressing TRPV4 in these animals remarkably increased body weight and fat mass by activating the S100a4/AMPKα signaling pathway, thereby promoting positive energy metabolism. Overexpressed hypothalamic TRPV4 impaired glucose tolerance, while promoting the accumulation of fat in liver cells, resulting in hepatic steatosis. In addition, the upregulation of hypothalamic TRPV4 reduces high-fat induced central inflammation. This study provides evidence that hypothalamic TRPV4 plays a significant role in regulating homeostasis. Hypothalamic TRPV4 emerges as a target for therapeutic intervention against obesity.

Adsorption of poly(oxyethylene) and hydroxyl group-containing nonionic surfactants on silica particles in NH4OH solution and its effect on the interaction force with Si surface

In the semiconductor manufacturing processes, surface cleaning is one of the most critical steps because particle contamination directly affects device yield. In addition, surface etching and oxidation should be minimized during the particle removal process. In this study, the dissolved oxygen concentration (DOC) in an NH4OH solution was reduced to suppress oxidation of Si. Additionally, nonionic surfactants were added to the solution to suppress the Si surface roughening and improve the particle removal efficiency in the NH4OH solution. Nonionic surfactant molecules were adsorbed on the Si surface, preventing the Si surface from attack by OH-. In addition, they were also adsorbed on the silica particle surfaces, producing repulsive hydration and osmotic forces between the adsorbed surfaces of the Si and silica particles while reducing the adhesion force between them. As a result, more than 95 % of particle removal efficiency and less than 0.6 nm of surface roughness were obtained when the particle-contaminated Si surface was treated with a low-DOC NH4OH solution containing a nonionic surfactant.

The Revised Starling Hypothesis: Modeling the impact of the glycocalyx on vascular refilling during ultrafiltration in humans

The glycocalyx lines systemic capillaries and influences the distribution of osmotic forces across the capillary between the intravascular and interstitial compartments. By creating a pericapillary space between the capillary and the interstitium with a low osmotic pressure, the predicted and measured water flux at the distal end of systemic capillaries is outward under physiological conditions – contrary to the prediction of the traditional Starling model of capillary fluid transport. This has led to a ‘revised’ Starling model in which the predicted the movement of water from the capillary into the interstitium is consistently outward, and the return of water from the interstitial compartment necessary to maintain intravascular volume occurs nearly exclusively through the lymphatic system. We developed a methematicl model of the revised Starling Hypothesis that is applicable to the whole body in the special circumstance of hemodialysis, where the contributions of renal function to blood volume regulation may be ignored, and the total input and output of water and solutes are controlled and measured as part of the process of hemodialysis. We created a revised, two compartment (vascular+interstitial space), Starling model using the quantitative model of Facchini et al. (Microvasc. Res. 94:52-63, 2014) that describes capillary transport through the glycocalyx (albeit as normalized dimensionless values). We modelled the return of interstitial water to the vascular space through lymphatic flow based on the interstitial pressure (Possenti et al., Micro. Vasc. Res. 122:101-110, 2019), and we estimated the interstitial pressure based upon the formulation of Chapple et al. (Comp. Meth, and Prog. In Biomed. 41: 33-54,1993). We used the two-compartment model (intravascular and extravascular spaces) developed by de los Reyes et al. (J. Theoret. Biol. 390:146-155, 2016) to analyze transcapillary fluxes based on the traditional Starling model, and we embedded the description of fluxes across glycocalyx developed by Facchini et al. to decribe the fluxes of solutes and water across the glycocalyx and peri-glycocalyx/sub-capillary space and added control of lymphatic function within this two-compartment model to create a revised Starling model. The traditional and revised models were evaluated using data from periods of ultrafiltration in which the hematocrit (Crit-line), body weight and measured fluid input or ultrafiltrate removed were measured, and we compared the predicted fluxes of solvent and solutes across the capillary and through the lymphatic system between the traditional and revised Starling models. The two models lead to dramatically different predictions—all of the fluid transported out of the capillary must come back via the lymphatics according to the revised Starling model. This places vital importance upon the lymphatic flow during vascular refilling when blood volume is reduced and must be repleted to maintain stable cardiac function. Partially funded by the Renal Research Institute This is the full abstract presented at the American Physiology Summit 2023 meeting and is only available in HTML format. There are no additional versions or additional content available for this abstract. Physiology was not involved in the peer review process.

An Insight into the Potassium Currents of hERG and Their Simulation.

By assuming that a stepwise outward movement of the four S4 segments of the hERG potassium channel determines a concomitant progressive increase in the flow of the permeant potassium ions, the inward and outward potassium currents can be simulated by using only one or two adjustable (i.e., free) parameters. This deterministic kinetic model differs from the stochastic models of hERG available in the literature, which usually require more than 10 free parameters. The K+ outward current of hERG contributes to the repolarization of the cardiac action potential. On the other hand, the K+ inward current increases with a positive shift in the transmembrane potential, in apparent contrast to both the electric and osmotic forces, which would concur in moving K+ ions outwards. This peculiar behavior can be explained by the appreciable constriction of the central pore midway along its length, with a radius < 1 Å and hydrophobic sacks surrounding it, as reported in an open conformation of the hERG potassium channel. This narrowing raises a barrier to the outward movement of K+ ions, inducing them to move increasingly inwards under a gradually more positive transmembrane potential.

Mitochondrial Cristae Morphology Reflecting Metabolism, Superoxide Formation, Redox Homeostasis, and Pathology.

Significance: Mitochondrial (mt) reticulum network in the cell possesses amazing ultramorphology of parallel lamellar cristae, formed by the invaginated inner mitochondrial membrane. Its non-invaginated part, the inner boundary membrane (IBM) forms a cylindrical sandwich with the outer mitochondrial membrane (OMM). Crista membranes (CMs) meet IBM at crista junctions (CJs) of mt cristae organizing system (MICOS) complexes connected to OMM sorting and assembly machinery (SAM). Cristae dimensions, shape, and CJs have characteristic patterns for different metabolic regimes, physiological and pathological situations. Recent Advances: Cristae-shaping proteins were characterized, namely rows of ATP-synthase dimers forming the crista lamella edges, MICOS subunits, optic atrophy 1 (OPA1) isoforms and mitochondrial genome maintenance 1 (MGM1) filaments, prohibitins, and others. Detailed cristae ultramorphology changes were imaged by focused-ion beam/scanning electron microscopy. Dynamics of crista lamellae and mobile CJs were demonstrated by nanoscopy in living cells. With tBID-induced apoptosis a single entirely fused cristae reticulum was observed in a mitochondrial spheroid. Critical Issues: The mobility and composition of MICOS, OPA1, and ATP-synthase dimeric rows regulated by post-translational modifications might be exclusively responsible for cristae morphology changes, but ion fluxes across CM and resulting osmotic forces might be also involved. Inevitably, cristae ultramorphology should reflect also mitochondrial redox homeostasis, but details are unknown. Disordered cristae typically reflect higher superoxide formation. Future Directions: To link redox homeostasis to cristae ultramorphology and define markers, recent progress will help in uncovering mechanisms involved in proton-coupled electron transfer via the respiratory chain and in regulation of cristae architecture, leading to structural determination of superoxide formation sites and cristae ultramorphology changes in diseases.

Single Hydrogel Particle Mechanics and Dynamics Studied by Combining Capillary Micromechanics with Osmotic Compression.

Hydrogels can exhibit a remarkably complex response to external stimuli and show rich mechanical behavior. Previous studies of the mechanics of hydrogel particles have generally focused on their static, rather than dynamic, response, as traditional methods for measuring single particle response at the microscopic scale cannot readily measure time-dependent mechanics. Here, we study both the static and the time-dependent response of a single batch of polyacrylamide (PAAm) particles by combining direct contact forces, applied by using Capillary Micromechanics, a method where particles are deformed in a tapered capillary, and osmotic forces are applied by a high molecular weight dextran solution. We found higher values of the static compressive and shear elastic moduli for particles exposed to dextran, as compared to water (KDex≈63 kPa vs. Kwater≈36 kPa, and GDex≈16 kPa vs. Gwater≈7 kPa), which we accounted for, theoretically, as being the result of the increased internal polymer concentration. For the dynamic response, we observed surprising behavior, not readily explained by poroelastic theories. The particles exposed to dextran solutions deformed more slowly under applied external forces than did those suspended in water (τDex≈90 s vs. τwater≈15 s). The theoretical expectation was the opposite. However, we could account for this behaviour by considering the diffusion of dextran molecules in the surrounding solution, which we found to dominate the compression dynamics of our hydrogel particles suspended in dextran solutions.

Bovine Serum Albumin Interaction with Polyanionic and Polycationic Brushes: The Case Theoretical Study.

We apply a coarse-grained self-consistent field Poisson-Boltzmann framework to study interaction between Bovine Serum Albumin (BSA) and a planar polyelectropyte brush. Both cases of negatively (polyanionic) and positively (polycationic) charged brushes are considered. Our theoretical model accounts for (1) re-ionization free energy of the amino acid residues upon protein insertion into the brush; (2) osmotic force repelling the protein globule from the brush; (3) hydrophobic interactions between non-polar areas on the globule surface and the brush-forming chains. We demonstrate that calculated position-dependent insertion free energy exhibits different patterns, corresponding to either thermodynamically favourable BSA absorption in the brush or thermodynamically or kinetically hindered absorption (expulsion) depending on the pH and ionic strength of the solution. The theory predicts that due to the re-ionization of BSA within the brush, a polyanionic brush can efficiently absorb BSA over a wider pH range on the "wrong side" of the isoelectric point (IEP) compared to a polycationic brush. The results of our theoretical analysis correlate with available experimental data and thus validate the developed model for prediction of the interaction patterns for various globular proteins with polyelectrolyte brushes.

Expansion microscopy through mechanical force.

In biophysics interesting phenomena take place during the interaction between biological molecules on the order of nanometers. Optical super-resolution imaging techniques surpass the diffraction limit of light enabling higher resolutions to study these phenomenon. However, super-resolution techniques usually require expensive equipment. Expansion microscopy (ExM) is a sample preparation method that facilitates super-resolution imaging by leveraging osmotic forces to physically separate features smaller than the diffraction limit of light. ExM is cheaper than and compatible with other super-resolution methods to reach the nanoscale. Currently, ExM commonly produces 4.5X linear expansion and 20X has been achieved using successive expansion steps, but this can result in fragmentation of the biological sample. Allowing the gel to absorb water to expand is also as low process. To overcome the fragmentation and time issues, here, we use a highly stretchable cross-linked polymer gel and a mechanical stretcher device to achieve similar 20X linear expansion in minutes. Since we do not rely on osmotic forces for the expansion, this method is more compatible with other techniques which are incompatible with excess water. We demonstrate our expansion microscopy method by imaging MOSE cells at 50 nm resolution. We establish mechanical force expansion microscopy as a viable sample preparation method with the same advantages as ExM while being much faster. This will also allow researchers to study time sensitive phenomenon.