Recent experiments by Kantsler et. al. (2007) have shown that the relaxational dynamics of a vesicle in external elongation flow is accompanied by the formation of wrinkles on a membrane. Motivated by these experiments we present a theory describing the dynamics of a wrinkled membrane. Formation of wrinkles is related to the dynamical instability induced by negative surface tension of the membrane. For quasi-spherical vesicles we perform analytical study of the wrinkle structure dynamics. We derive the expression for the instability threshold and identify three stages of the dynamics. The scaling laws for the temporal evolution of wrinkling wavelength and surface tension are established and confirmed numerically.
We present experimental results on the relaxation dynamics of vesicles subjected to a time-dependent elongation flow. We observed and characterized a new instability, which results in the formation of higher order modes of the vesicle shape (wrinkles), after a switch in the direction of the gradient of the velocity. This surprising generation of membrane wrinkles can be explained by the appearance of a negative surface tension during the vesicle deflation, due to compression in a sign-switching transient. Moreover, the formation of buds in the vesicle membrane has been observed in the vicinity…
Tank-treading, tumbling and trembling are different types of the vesicle behavior in an external flow. We derive a dynamical equation for nearly spherical vesicles enabling to establish a phase diagram of the system predicting the regimes. The diagram is drawn in terms of two dimensionless parameters depending on the vesicle excess area, fluid viscosities, membrane viscosity and bending modulus, strength of the flow, and ratio of the elongational and rotational components of the flow. The tank-treading to tumbling transition occurs via a saddle-node bifurcation whereas the tank-treading to tre…
We analytically derive an equation describing vesicle evolution in a fluid where some stationary flow is excited regarding that the vesicle shape is close to a sphere. A character of the evolution is governed by two dimensionless parameters, $S$ and $Λ$, depending on the vesicle excess area, viscosity contrast, membrane viscosity, strength of the flow, bending module, and ratio of the elongation and rotation components of the flow. We establish the ``phase diagram'' of the system on the $S-Λ$ plane: we find curves corresponding to the tank-treading to tumbling transition (described by the sadd…
Renormalized mechanics and stochastic thermodynamics of growing vesicles
The James Franck Institute, University of Chicago（芝加哥大学詹姆斯·弗兰克研究所）；Department of Chemistry, University of Chicago（芝加哥大学化学系）；Engineering Sciences and Applied Mathematics, Northwestern University（西北大学工程科学与应用数学系）
The dynamics and rheology of suspensions of fluid vesicles or red blood cells is investigated by a combination of molecular dynamics and mesoscale hydrodynamics simulations in two dimensions. The vesicle suspension is confined between two no-slip walls, which are driven externally to generate a shear flow with shear rate $\dotγ$. The flow behavior is studied as a function of $\dotγ$, the volume fraction of vesicles, and the viscosity contrast between inside and outside fluids. Results are obtained for the encounter and interactions of two vesicles, the intrinsic viscosity of the suspension, an…
We review the dynamical behavior of giant fluid vesicles in various types of external hydrodynamic flow. The interplay between stresses arising from membrane elasticity, hydrodynamic flows, and the ever present thermal fluctuations leads to a rich phenomenology. In linear flows with both rotational and elongational components, the properties of the tank-treading and tumbling motions are now well described by theoretical and numerical models. At the transition between these two regimes, strong shape deformations and amplification of thermal fluctuations generate a new regime called trembling. I…
Numerical simulations of vesicle suspensions are performed in two dimensions to study their dynamical and rheological properties. An hybrid method is adopted, which combines a mesoscopic approach for the solvent with a curvature-elasticity model for the membrane. Shear flow is induced by two counter-sliding parallel walls, which generate a linear flow profile. The flow behavior is studied for various vesicle concentrations and viscosity ratios between the internal and the external fluid. Both the intrinsic viscosity and the thickness of depletion layers near the walls are found to increase wit…
The migration of a suspended vesicle in an unbounded Poiseuille flow is investigated numerically in the low Reynolds number limit. We consider the situation without viscosity contrast between the interior of the vesicle and the exterior. Using the boundary integral method we solve the corresponding hydrodynamic flow equations and track explicitly the vesicle dynamics in two dimensions. We find that the interplay between the nonlinear character of the Poiseuille flow and the vesicle deformation causes a cross-streamline migration of vesicles towards the center of the Poiseuille flow. This is in…
The external electric field deforms flaccid phospholipid vesicles into spheroidal bodies, with the rotational axis aligned with its direction. Deformation is frequency dependent: in the low frequency range (~ 1 kHz), the deformation is typically prolate, while increasing the frequency to the 10 kHz range changes the deformation to oblate. We attempt to explain this behaviour with a theoretical model, based on the minimization of the total free energy of the vesicle. The energy terms taken into account include the membrane bending energy and the energy of the electric field. The latter is calcu…
Recent studies of elasto-capillary phenomena have triggered interest in a basic variant of the classical Young-Laplace-Dupré (YLD) problem: The capillary interaction between a liquid drop and a thin solid sheet of low bending stiffness. Here, we consider a two-dimensional model where the sheet is subjected to an external tensile load and the drop is characterized by a well-defined Young's contact angle $θ_Y$. Using a combination of numerical, variational, and asymptotic techniques, we discuss wetting as a function of the applied tension. We find that, for wettable surfaces with $0<θ_Y<π/2$, co…
Biological membranes constantly change their shape in response to external stimuli, and understanding the remodeling and stability of vesicles in heterogeneous environments is therefore of fundamental importance for a range of cellular processes. One crucial question is how vesicles respond to external osmotic stresses, imposed by differences in solute concentrations between the vesicle interior and exterior. Previous analyses of the membrane bending energy have predicted that micron-sized giant unilamellar vesicles (GUVs) should become globally deformed already for nanomolar concentration dif…
When the charge densities on the inner and outer surface of the vesicle membrane are similar one may assume that the potential at a point closer to the outer/inner surface is more affected by the charges located at the outer/inner surface of the vesicle membrane. However, because of the curvature of the vesicle and the screening effect of the electrolyte ions the situation is more complicated. When the charge densities at the inner and outer surface of the vesicle membrane are the same then at any finite distance Z from the center of the vesicle the contribution of the charges, located at the …
We show that a spontaneous bending of single layer bolaamphiphiles results from the frustration due to the competition between core-core and tail-solvent interactions. We find that spherical vesicles are stable under rather general assumptions on these interactions described within the Flory-Huggins theory. We consider also the deformation of the vesicles in an external magnetic field that has been recently experimentally observed.
Lipid bilayer membranes have a native (albeit small) permeability for water molecules. Under an external load, provided that the bilayer structure stays intact and does not suffer from poration or rupture, a lipid membrane deforms and its water influx/efflux is often assumed negligible in the absence of osmolarity. In this work we use boundary integral simulations to investigate the effects of water permeability on the vesicle hydrodynamics due to a mechanical load, such as the viscous stress from an external flow deforming a vesicle membrane in free space or pushing it through a confinement. …
A phase field model for dealing with shape instabilities in fluid membrane vesicles is presented. This model takes into account the Canham-Helfrich bending energy with spontaneous curvature. A dynamic equation for the phase-field is also derived. With this model it is possible to see the vesicle shape deformation dynamically, when some external agent instabilizes the membrane, for instance, inducing an inhomogeneous spontaneous curvature. The numerical scheme used is detailed and some stationary shapes are shown together with a shape diagram for vesicles of spherical topology and no spontaneou…
The morphology of spherically confined flexoelectric fluid membrane vesicles in an external uniform electric field is studied numerically. Due to the deformations induced by the confinement, the membrane becomes polarized resulting in an interaction with the external field. The equilibrium shapes of the vesicle without electric field can be classified in a geometrical phase diagram as a function of scaled area and reduced volume [1,2]. When the area of the membrane is only slightly larger than the area of the confining sphere, a single axisymmetric invagination appears. A non-vanishing electri…
Using a microfluidic trap, we study the behavior of individual phospholipid vesicles in contact with fatty acids. We show that spontaneous fatty acids insertion inside the bilayer is controlled by the vesicle size, osmotic pressure difference across the membrane and fatty acids concentration in the external bath. Depending on these parameters, vesicles can grow spherically or become unstable and fragment into several daughter vesicles. We establish the phase diagram for vesicle growth and we derive a simple thermodynamic model that reproduces the time evolution of the vesicle volume. Finally, …
We present rheology experiments on dilute solutions of vesicles and red blood cells (RBC). Varying the viscosity ratio $λ$ between internal and external fluids, the microscopic dynamics of suspended objects can be qualitatively changed from tank-treading ($tt$) to tumbling ($tb$). We find that in the tt regime the viscosity $η$, decreases when $λ$ increases, in contrast with droplet emulsions and elastic capsule theories which are sometimes invoked to model RBC dynamics. At a critical $λ$ (close to the tt-tb transition) $η$ exhibits a minimum before it increases in the tb regime. This is consi…
The dynamics of a single fluid bilayer membrane in an external hydrodynamic flow field is considered. The deterministic equation of motion for the configuration is derived taking into account both viscous dissipation in the surrounding liquid and local incompressibility of the membrane. For quasi-spherical vesicles in shear flow, thermal fluctuations can be incorporated in a Langevin-type equation of motion for the deformation amplitudes. The solution to this equation shows an overdamped oscillatory approach to a stationary tanktreading shape. Inclination angle and ellipiticity of the contour …
The use of tank-treading as a means of propulsion for microswimmers in viscous shear flows is taken into exam. We discuss the possibility that a vesicle be able to control the drift in an external shear flow, by varying locally the bending rigidity of its own membrane. By analytical calculation in the quasi-spherical limit, the stationary shape and the orientation of the tank-treading vesicle in the external flow, are determined, working to lowest order in the membrane inhomogeneity. The membrane inhomogeneity acts in the shape evolution equation as an additional force term, that can be used t…
Osmotic deflation of vesicles enclosing two liquid phases can lead to bulging of one of the phases from the vesicle body. This budding process is preceded by a complete to partial wetting transition of one of the liquid phases on the membrane and depends on the membrane tensions and the tension of the interface between the enclosed liquid phases. These tensions dominate in different morphology regimes, the crossover of which initiates the budding process. In addition, the degree of budding can be controlled by aspiration via micropipettes. We also demonstrate that the budding direction can be …
Osmotically Induced Shape Changes in Membrane Vesicles
Kansas State University（堪萨斯州立大学）；NewOrbit Space Ltd（NewOrbit空间有限公司）；University of Sheffield（谢菲尔德大学）；Kaplan International College（凯伦国际学院）；Université Paris-Saclay（巴黎萨克雷大学）
We present a hybrid simulation method which allows one to study the dynamical evolution of self-assembling (co)polymer solutions in the presence of hydrodynamic interactions. The method combines an established dynamic density functional theory for polymers that accounts for the nonlocal character of chain dynamics at the level of the Rouse model, the external potential dynamics (EPD) model, with an established Navier-Stokes solver, the Lattice Boltzmann (LB) method. We apply the method to study the self-assembly of nanoparticles and vesicles in two-dimensional copolymer solutions in a typical …
Lipid bilayer membranes are the fundamental biological barriers that permit life. The bilayer dynamics largely participates in orchestrating cellular workings and is characterized by substantial stability together with extreme plasticity that allows controlled morphological/topological changes. Modeling and understanding the topological change of vesicle-like membrane at the scale of a full cell has proved an elusive aim. We propose and discuss here a continuum model able to encompass the fusion/fission transition of a bilayer membrane at the scale of a Large Unilamellar Vesicle and evaluate t…
Despite its significance in microfluidics, the effect of confinement on the transition from the tank-treading (steady motion) to the tumbling (unsteady motion) dynamical state of deformable micro-particles has not been studied in detail. In this paper, we investigate the dynamics of a single viscous vesicle under confining shear as a general model system for red blood cells, capsules, or viscous droplets. The transition from tank-treading to tumbling motion can be triggered by the ratio between internal and external fluid viscosities. Here, we show that the transition can be induced solely by …
An exact description is provided of an almost spherical fluid vesicle with a fixed area and a fixed enclosed volume locally deformed by external normal forces bringing two nearby points on the surface together symmetrically. The conformal invariance of the two-dimensional bending energy is used to identify the distribution of energy as well as the stress established in the vesicle. While these states are local minima of the energy, this energy is degenerate; there is a zero mode in the energy fluctuation spectrum, associated with area and volume preserving conformal transformations, which brea…
In most practical situations, active particles are affected by their environment, for example, by a chemical concentration gradient, light intensity, gravity, or confinement. In particular, the effect of an external flow field is important for particles swimming in a solvent fluid. For deformable active particles such as self-propelled liquid droplets and active vesicles, as well as microorganisms such as euglenas and neutrophils, a general description has been developed by focusing on shape deformation. In this review, we present our recent studies concerning the dynamics of a single active d…
Salt is a very common molecule in aqueous environments but the question of whether the interactions of monovalent ions Na^+ and Cl^- ,with the neutral heads of phospholipids are impactful enough to change the membrane rigidity is still a mystery. To provide a resolution to this long simmering debate, we investigated the dynamics of DOPC vesicles in the fluid phase with increasing external salt concentration. At higher salt concentrations, we observe an increase in bending rigidity from neutron spin echo spectroscopy (NSE) and an increase in bilayer thickness from small-angle X-ray scattering (…
The possibility of microscopic swimming by extraction of energy from an external flow is discussed, focusing on the migration of a simple trimer across a linear shear flow. The geometric properties of swimming, together with the possible generalization to the case of a vesicle, are analyzed.The mechanism of energy extraction from the flow appears to be the generalization to a discrete swimmer of the tank-treading regime of a vesicle. The swimmer takes advantage of the external flow by both extracting energy for swimming and "sailing" through it. The migration velocity is found to scale linearl…
The presence of membrane tubules in living cells is essential to many biological processes. In cells, one mechanism to form nanosized lipid tubules is via molecular motor induced bilayer extraction. In this paper, we describe a simple experimental model to investigate the forces required for lipid tube formation using kinesin motors anchored to DOPC vesicles. Previous related studies have used molecular motors actively pulling on the membrane to extract a nanotube. Here, we invert the system geometry; molecular motors are used as static anchors linking DOPC vesicles to a two-dimensional microt…
Calcein leakage assays are a standard experimental set-up for probing the extent of damage induced by external agents on synthetic lipid vesicles. The fluorescence signal associated with calcein release from liposomes is the signature of vesicle disruption, transient pore formation or vesicle fusion. This type of assay is widely used to test the membrane disruptive effect of biological macromolecules, such as proteins, antimicrobial peptides and RNA and is also used on synthetic nanoparticles with a polymer, metal or oxide core. Little is known about the effect that calcein and other fluoresce…
Whilst many vertebrates appear externally left-right symmetric, the arrangement of internal organs is asymmetric. In zebrafish, the breaking of left-right symmetry is organised by Kupffer's Vesicle (KV): an approximately spherical, fluid-filled structure that begins to form in the embryo 10 hours post fertilisation. A crucial component of zebrafish symmetry breaking is the establishment of a cilia-driven fluid flow within KV. However, it is still unclear (a) how dorsal, ventral and equatorial cilia contribute to the global vortical flow, and (b) if this flow breaks left-right symmetry through …
The self-assembly of copolymeric vesicles and micelles in micromixers is studied by External Potential Dynamics (EPD) simulations -- a dynamic density functional approach that explicitly accounts for the polymer architecture both at the level of thermodynamics and dynamics. Specifically, we focus on the co-solvent method, where nanoparticle precipitation is triggered by mixing a poor co-solvent into a homogeneous copolymer solution in a micromixer. Experimentally, it has been reported that the flow rate in the micromixers influences the size of the resulting particles as well as their morpholo…
We study a dynamical curvature instability caused by a local chemical modification of a phospholipid membrane. In our experiments, a basic solution is microinjected close to a giant unilamellar vesicle, which induces a local chemical modification of some lipids in the external monolayer of the membrane. This modification causes a local deformation of the vesicle, which then relaxes. We present a theoretical description of this instability, taking into account both the change of the equilibrium lipid density and the change of the spontaneous membrane curvature induced by the chemical modificati…
Cell plasma membranes display a dramatically rich structural complexity characterized by functional sub-wavelength domains with specific lipid and protein composition. Under favorable experimental conditions, patterned morphologies can also be observed in vitro on model systems such as supported membranes or lipid vesicles. Lipid mixtures separating in liquid-ordered and liquid-disordered phases below a demixing temperature play a pivotal role in this context. Protein-protein and protein-lipid interactions also contribute to membrane shaping by promoting small domains or clusters. Such phase s…
We calculate the fluctuation spectrum of the shape of a lipid vesicle or cell exposed to a nonthermal source of noise. In particular we take into account constraints on the membrane area and the volume of fluid that it encapsulates when obtaining expressions for the dependency of the membrane tension on the noise. We then investigate three possible origins of the non-thermal noise taken from the literature: A direct force, which models an external medium pushing on the membrane. A curvature force, which models a fluctuating spontaneous curvature, and a permeation force coming from an active tr…
The optimal strategy for a microscopic swimmer to migrate across a linear shear flow is discussed. The two cases, in which the swimmer is located at large distance, and in the proximity of a solid wall, are taken into account. It is shown that migration can be achieved by means of a combination of sailing through the flow and swimming, where the swimming strokes are induced by the external flow without need of internal energy sources or external drives. The structural dynamics required for the swimmer to move in the desired direction is discussed and two simple models, based respectively on th…
