Multiparticle Collision Dynamics Research Articles

Particle-based mesoscopic model for phase separation in a binary fluid mixture.

A mesoscopic simulation model to study the phase separation in a binary fluid mixture in three dimensions (3D) is presented here by augmenting the existing particle-based multiparticle collision dynamics (MPCD) algorithm. The approach describes the nonideal equationof the fluid state by incorporating the excluded-volume interaction between the two components within the framework of stochastic collision, which depends on the local fluid composition and velocity. Calculating the nonideal contribution to the pressure both from simulation and analytics shows the model to be thermodynamically consistent. A phase diagram to explore the range of parameters that give rise to phase separation in the model is investigated. The interfacial width and phase growth obtained from the model agree with the literature for a wide range of temperatures and parameters.

Confined Electrolytes Show Bulk Dynamics Modulated by Hydrodynamic Couplings with the Walls

We use numerical simulations at the mesoscopic scale, namely, multiparticle collision dynamics (MPCD), to investigate the properties of electrolyte solutions in a charged slit pore. The solution is described within the primitive model of electrolytes, where ions are charged hard spheres embedded in a dielectric medium. Hydrodynamic couplings between ions and with the charged walls are precisely accounted for by the MPCD algorithm. We show that the dynamic properties of ions in this situation strongly differ from the behavior at infinite dilution (ideal case), contrary to what is usually assumed in the usual Poisson-Nernst-Planck description of this kind of systems. As a consequence of confinement, the diffusion coefficients of ions unexpectedly increase with the average ionic density in the systems. This is due to a decrease of the proportion of ions that are slowed down by the wall. Moreover, nonequilibrium simulations are used to estimate the electrical conductivity of these confined electrolytes. We show that the simulation results can be accounted for quantitatively by combining bulk descriptions of the electrical conductivity of electrolytes with a simple description of the hydrodynamics of ions in a slit pore.

Behaviors of a Polymer Chain in Channels: From Zimm to Rouse Dynamics

The effects of confinement and hydrodynamic interactions on single-chain diffusion behaviors are studied by using a combination of molecular dynamics and multiparticle collision dynamics simulations. For polymers in free space, the simulation results showed that the diffusion coefficient D∞ for long chains scales with the chain length N as D∞ ∼ N–ν (ν = 0.588), consistent with the Zimm dynamics, but it deviates from the Zimm dynamics for short chains. For polymers confined in channels with width H, the diffusion coefficient is found to follow two different scaling relations. The observed behaviors could be understood by introducing a microscopic hydrodynamic length ξh, below which the overall effect of hydrodynamic interactions becomes less important. For a confined chain, the diffusion behavior exhibits a crossover from Zimm (nondraining) to Rouse (free draining) dynamics as the channel size H decreases. When H is larger than ξh, the confinement experienced by the polymer chain is weak and the diffusion coefficient scales as D ∼ H0.7, in accordance with the prediction of blob theory; when H is smaller than ξh, D becomes independent of H, implying a free draining condition. A general analytical expression of D is derived by extending the partially permeable sphere model to the blob scale, which gives a quantitative description of the transition from Zimm to Rouse dynamics as H decreases.

What quantity of charge on the nanoparticle can result in a hybrid morphology of the nanofluid and a higher thermal conductivity?

One of the most important mechanisms for promotion of the thermal conductivity(TC) of nanofluid is aggregation of nanoparticles. In present work, a hybrid method of multi-particle collision dynamics and molecular dynamics (MPCD-MD) is employed to evaluate the aggregation morphology and TC of Cu-H2O nanofluid. Numerical simulations for various quantity of charges (QoC) on nanoparticles are conducted, and three kinds of morphology of nanoparticles distribution, whole aggregation morphology at lower QoC, hybrid morphology at moderate QoC and fully dispersed morphology at greater QoC, are obtained for the first time in microscopic simulations. For hybrid morphologies, the fractal dimension first drops and then rises with increasing QoC, since aggregates can break up into several clusters at relatively low QoC and can be fully dispersed at relatively high QoC. Instead, the TC first increases and then decreases, and the TC can reach a peak at a certain QoC. The underneath mechanism should be a balance between the effects of nanolayers and Kapitza resistance. This can provide helpful guidance to prepare nanofluids with higher TC.

Dynamics of semi‐flexible and breakable fibers under Poiseuille flow

AbstractIn the processing of fiber‐reinforced polymer composites, especially in injection molding, the fiber's orientation, length, and distribution vary depending on the location of the channel flow and its properties, which affects the performance of final products. To investigate the intricate behavior of fiber suspensions under Poiseuille flow, we used the hybrid simulation approach, multiparticle collision dynamics–molecular dynamics (MPC‐MD), which takes hydrodynamic interactions and fiber properties (strength, flexibility) into account. For non‐breakable and rodlike fibers, fibers align well along the flow direction while showing more alignment near the wall. As fiber becomes breakable and/or flexible, the length and orientation of fibers strongly depend on their properties. The interesting phenomenon is specifically seen for breakable and semiflexible fibers, where the orientation of the fiber exhibits non‐monotonic behavior depending on the flow rate. This complex behavior highlights the importance of comprehending the dynamics of many types of fibers and necessitates research into the best conditions for injection molding.

Structure and dynamics of chemically active ring polymers: swelling to collapse.

The ring structures are common in many synthetic or natural systems and experience both local and long-range forces by chemical sensing. This work is an effort to investigate the structural and dynamical properties of a chemically active ring in an explicit solvent bath utilizing hybrid molecular dynamics (MD) and multiparticle collision dynamics (MPCD) simulation techniques. We show that by tuning the chemical properties of the ring, it can be converted from a chemo-attractant to a chemo-repellent, thereby changing the steady state to be either collapsed or swelled as compared to its passive limit. We quantify these observations by comparing the scaling laws, local structures and the dynamics of active and passive rings. Furthermore, we show the impact of varying numbers of active sites by calculating the contact probability of the collapse state that highlights diverse structures. We also analyze the dynamics of the ring by finding the relaxation time and the mean square displacement of the centre of mass. A faster relaxation with enhanced diffusion is observed for the active rings.

Active nematic liquid crystals simulated by particle-based mesoscopic methods.

Two Multi-particle collision dynamics algorithms that simulate nematic liquid crystals are generalised to reproduce active behaviour. One of the algorithms is due to Shendruk and Yeomans and is based on particles that carry an orientation vector ordered by a mean-field energy [T. N. Shendruk and J. M. Yeomans, Soft Matter, 2015, 11, 5101]. In the other algorithm, due to Mandal and Mazza, particles possess an order parameter tensor which evolves according to the Qian-Sheng model of nematohydrodynamics [S. Mandal and M. G. Mazza, Phys. Rev. E, 2019, 99, 063319]. For both methods activity is incorporated through a force proportional to the divergence of the local average order parameter tensor. Both implementations produce disclination curves in the nematic fluid that undergo nucleation and self-annihilation dynamics. Topological defects are found to be consistent with those observed in recent experiments of three-dimensional active nematics. Results permit to compare the length-scales over which the different nematic Multi-particle collision dynamics methods operate. The structure and dynamics of the orientation and flow fields agree with those obtained recently in numerical studies of continuum three-dimensional active nematics. Overall, our results open the opportunity to use mesoscopic particle-based approaches to study active liquid crystals in situations such as nonequilibrium states driven by flow or colloidal particles in active anisotropic solvents.

Single-polymer dynamics of starch-like branched ring polymers in steady shear flow

The stretching dynamics and dynamical behaviors of individual branched ring polymer (BRP), a coarse-grained model for some types of the starch, in steady shear flow are studied by using a hybrid mesoscale simulation approach that combines multiparticle collision dynamics with standard molecular dynamics. By analyzing the stretched configuration of BRPs, we find the polymer size increases nonmonotonically with increasing branch length. Meanwhile, the decrease of the alignment angle of the stretched configuration of BRPs follows a universal power law during the first downward phase as the shear rate increases. Constructing the three-dimensional surface of the polymer's ring backbone and tracing the temporal fluctuations of the surface's normal vector along the simulation trajectory, the tumbling and tank-treading motion are clearly reflected by periodic and non-periodic changes of the normal vector. Interestingly, these temporal changes are much more regular than that of the gyration tensor. Thus, a novel cross-correlation function, which is the correlation between fluctuations of the normal vector along the flow direction and the velocity-gradient direction, is proposed to analyze the tumbling motion that usually coexists with the tank-treading motion. This function can naturally address the fails of traditional method that analyzing the tumbling motion by determining the correlation of temporal fluctuations of the gyration tensor Gαα. By analyzing the dynamical behaviors of BRPs, diverse dependences of the tumbling frequency ωTB and tank-treading frequency ωTT on the shear rate γ̇ are observed at a wide range of shear rates and polymer sizes. Furthermore, our simulations also reveal that the tank-treading motion is more stable than the tumbling motion for small-branch-size BRPs but the tumbling motion is more stable than the tank-treading motion for large-branch-size BRPs.

Simulating the flow of interacting ferrofluids with multiparticle collision dynamics.

Ferrofluid flow is fascinating since its fluid properties can conveniently be manipulated by external magnetic fields. Novel applications in micro- and nanofluidics as well as in biomedicine have renewed the interest in the flow of colloidal magnetic nanoparticles with a focus on small-scale behavior. Traditional flow simulations of ferrofluids, however, often use simplified constitutive models and do not include fluctuations that are relevant at small scales. Here we address these challenges by proposing a hybrid scheme that combines the multiparticle collision dynamics method for modeling hydrodynamics with Brownian dynamics simulations of a reliable kinetic model describing the microstructure, magnetization dynamics, and resulting stresses. Since both multiparticle collision dynamics and Brownian dynamics are mesoscopic methods that naturally include fluctuations, this hybrid scheme presents a promising alternative to more traditional approaches, also because of the flexibility to model different geometries and modifying the constitutive model. The scheme was tested in several ways. Poiseuille flow was simulated for various model parameters and effective viscosities were determined from the resulting flow profiles. The effective, field-dependent viscosities are found to be in very good agreement with theoretical predictions. We also study Stokes' second flow problem for ferrofluids. For weak amplitudes and low frequencies of the oscillating plate, we find that the velocity profiles are well described by the result for Newtonian fluids at the corresponding, field-dependent viscosity. Furthermore, the time-dependent profiles of the nonequilibrum magnetization component are well approximated by their steady-state values in stationary shear when evaluated with the instantaneous local shear rate. Finally, we also apply our scheme to simulate ferrofluid shear flow over a rough surface. We find characteristic differences in the nonequilibrium magnetization components when the external field is oriented in flow and in a gradient direction.

Negative differential thermal resistance of fluids induced by heat baths

It has recently been shown that in one-dimensional hard-point gases, there is a mechanism that induces negative differential thermal resistance (NDTR) between heat baths. We examine this mechanism in more general higher-dimensional fluids described by multiparticle collision dynamics. We consider fluids in a finite cuboid region of three-dimensional space with each end in contact with a heat bath. Based on analytical results and numerical models, we find that the mechanism underlying NDTR also works for high-dimensional fluidic systems with weak interactions and is very robust to mixed fluids. Our results significantly advance knowledge of NDTR induced by heat baths and illuminate different directions to explore in fabricating fluid thermal transistors in micro- and nanosystems.

Dynamical and Structural Properties of Comb Long-Chain Branched Polymer in Shear Flow.

Using hybrid multi-particle collision dynamics (MPCD) and a molecular dynamics (MD) method, we investigate the effect of arms and shear flow on dynamical and structural properties of the comb long-chain branched (LCB) polymer with dense arms. Firstly, we analyze dynamical properties of the LCB polymer by tracking the temporal changes on the end-to-end distance of both backbones and arms as well as the orientations of the backbone in the flow-gradient plane. Simultaneously, the rotation and tumbling behaviors with stable frequencies are observed. In other words, the LCB polymer undergoes a process of periodic stretched–folded–stretched state transition and rotation, whose period is obtained by fitting temporal changes on the orientation to a periodic function. In addition, the impact induced by random and fast motions of arms and the backbone will descend as the shear rate increases. By analyzing the period of rotation behavior of LCB polymers, we find that arms have a function in keeping the LCB polymer’s motion stable. Meanwhile, we find that the rotation period of the LCB polymer is mainly determined by the conformational distribution and the non-shrinkable state of the structure along the velocity-gradient direction. Secondly, structural properties are numerically characterized by the average gyration tensor of the LCB polymer. The changes in gyration are in accordance with the LCB polymer rolling when varying the shear rate. By analyzing the alignment of the LCB polymer and comparing with its linear and star counterparts, we find that the LCB polymer with very long arms, like the corresponding linear chain, has a high speed to reach its configuration expansion limit in the flow direction. However, the comb polymer with shorter arms has stronger resistance on configuration expansion against the imposed flow field. Moreover, with increasing arm length, the comb polymer in shear flow follows change from linear-polymer-like to capsule-like behavior.

Mesoscopic simulations of active nematics.

Coarse-grained, mesoscale simulations are invaluable for studying soft condensed matter because of their ability to model systems in which a background solvent plays a substantial role but is not the primary interest. Such methods generally model passive solvents; however, far-from-equilibrium systems may also be composed of complex solutes suspended in an active fluid. Yet, few coarse-grained simulation methods exist to model an active medium. We introduce an algorithm to simulate active nematics, which builds on multiparticle collision dynamics (MPCD) for passive fluctuating nematohydrodynamics by introducing dipolar activity in the local collision operator. Active nematic MPCD (AN-MPCD) simulations not only exhibit the key characteristics of active nematic turbulence but, as a particle-based algorithm, also reproduce crucial attributes of active particle models. Thus, mesoscopic AN-MPCD is an approach that bridges microscopic and continuum descriptions, allowing simulations of composite active-passive systems.

Regime change in the aggregate structure of magnetic disk-like particles in a quasi-2D suspension system via multi-particle collision dynamics simulations

We have addressed the problem of controlling a regime change in a quasi-2D system of magnetic disk-like particles by means of the strength and direction of an applied magnetic field. In the present study, two typical directions have been addressed, i.e. a y-direction field parallel to the 2D plane and a z-direction field normal to that plane of the particle disk. It is shown that the direction of an applied magnetic field is a significant factor in particle aggregation and can give rise to different regime changes. That is, an applied magnetic field parallel to the 2D system plane functions to induce a regime change in the aggregate structure from linear column-like particle clusters into a knitting-pattern formation, whereas in the case of an applied field normal to the 2D plane, a regime of long column-like clusters transforms into a particle distribution with no discernible internal structure. Key points of the present paper: The direction of an applied magnetic field may give rise to significantly different regime changes in particle aggregation. An applied magnetic field parallel to the 2D system plane induces a regime change from long linear column-like clusters into a knitting-pattern formation. A magnetic field in a direction normal to the 2D plane induces a regime change from long linear column-like clusters into a regime with no discernible internal structure. The strength and the direction of an applied magnetic field is a feasible tool for controlling a regime change in the aggregate structure.

Effect of amplitude and wavelength in the cooperative motion of Taylor lines

In the present study, we have modeled the clustering of binary Taylor line swimmers in a Newtonian fluid. The fluid is modeled using the particle-based simulation method multiparticle collision dynamics, while for the Taylor line, we use a bead spring arrangement with a sine wave passing through it using a bending wave potential. The binary swimmers have the same propulsion speed, but they differ from each other in the shape of the Taylor line ensured by different amplitudes and lengths. We observe that an optimal amplitude exists for the Taylor line swimmer leading to large clusters formation. The size distribution of the clusters was observed to follow a power-law behavior followed by an exponential cutoff. We also calculated the probability of finding a bead of the swimmer as a function of the fractional distance from the center of the bounding circle and observed that when the amplitude is close to the optimal value, the swimmer forms clusters closer to the walls; otherwise, the swimmer stays almost uniformly distributed around the bounding area. When the ratio of the amplitude is high, the clusters formed at the center of the bounding area become stable and have a wedge-shape. By calculating the speed of the swimmer as a function of the fractional distance from the center of the bounding area, we show that the swimmers speed increases with the maximum at the walls. The simulation with a smaller system has revealed that the maximum clustering happens for an amplitude parameter of ∼0.17.

Alignment and propulsion of squirmer pusher-puller dumbbells.

The properties of microswimmer dumbbells composed of pusher-puller pairs are investigated by mesoscale hydrodynamic simulations employing the multiparticle collision dynamics approach for the fluid. An individual microswimmer is represented by a squirmer, and various active-stress combinations in a dumbbell are considered. The squirmers are connected by a bond, which does not impose any geometrical restriction on the individual rotational motion. Our simulations reveal a strong influence of the squirmers' flow fields on the orientation of their propulsion directions, their fluctuations, and the swimming behavior of a dumbbell. The properties of pusher-puller pairs with an equal magnitude of the active stresses depend only weakly on the stress magnitude. This is similar to dumbbells of microswimmers without hydrodynamic interactions. However, for non-equal stress magnitudes, the active stress implies strong orientational correlations of the swimmers' propulsion directions with respect to each other, as well as the bond vector. The orientational coupling is most pronounced for pairs with large differences in the active-stress magnitude. The alignment of the squirmers' propulsion directions with respect to each other is preferentially orthogonal in dumbbells with a strong pusher and weak puller, and antiparallel in the opposite case when the puller dominates. These strong correlations affect the active motion of dumbbells, which is faster for strong pushers and slower for strong pullers.

Mechanisms of Flow-Induced Polymer Translocation

Flow-induced translocation of linear and ring polymers is studied by using a combination of multiparticle collision dynamics and molecular dynamics. The results show that both end capture and fold capture are present in the capture process of linear chains in weak flows, whereas fold capture becomes dominant in strong flows, resulting in similar behavior for the linear and ring chains in the strong flow regime. For narrow channels, the critical flux decreases with the increase of channel size, which is qualitatively consistent with the prediction by Wu et al.; for large channel sizes (which are still smaller than the polymer size), the critical flux is independent of channel size, in agreement with an earlier prediction by de Gennes et al. The presence of these two scaling regimes indicates that the confined blob exhibits a crossover from free draining to nondraining as the channel size increases. Moreover, we found that the conformation of the polymer exhibits a flow-induced coil–compact–stretch transition, and the transition does not appear to be first order. In addition, we observed that the monomers far from the channel and in the channel exhibit independent dynamics.

Multiparticle collision dynamics for ferrofluids.

Detailed studies of the intriguing field-dependent dynamics and transport properties of confined flowing ferrofluids require efficient mesoscopic simulation methods that account for fluctuating ferrohydrodynamics. Here, we propose such a new mesoscopic model for the dynamics and flow of ferrofluids, where we couple the multi-particle collision dynamics method as a solver for the fluctuating hydrodynamics equations to the stochastic magnetization dynamics of suspended magnetic nanoparticles. This hybrid model is validated by reproducing the magnetoviscous effect in Poiseuille flow, obtaining the rotational viscosity in quantitative agreement with theoretical predictions. We also illustrate the new method for the benchmark problem of flow around a square cylinder. Interestingly, we observe that the length of the recirculation region is increased, whereas the drag coefficient is decreased in ferrofluids when an external magnetic field is applied compared with the field-free case at the same effective Reynolds number. The presence of thermal fluctuations and the flexibility of this particle-based mesoscopic method provide a promising tool to investigate a broad range of flow phenomena of magnetic fluids, and the method could also serve as an efficient way to simulate solvent effects when colloidal particles are immersed in ferrofluids.

A Trefoil Knot Polymer Chain Translocates through a Funnel-like Channel: A Multi-Particle Collision Dynamics Study.

With combining multi-particle collision dynamics (MPCD) for the solvent and molecular dynamics (MD) for the polymer chains, we have studied the conformation and untying behaviors of a trefoil knot polymer chain translocated through a confined funnel-like channel. For the trefoil knot chain, we found that the untying knot behavior mostly happens during the translocation process, and the translocation behavior of linear chains is also simulated as a comparison. Some characteristics of the trefoil knot chain during translocation process, such as average gyration radius <Rg> and the average end-to-end distances <S> are discussed, and we statistic the scale relations of the translocation time versus the chain length, and that of the chain rigidity. This study may help to understand translocation behaviors of the knotted linear polymer chain in the capillary flow field.

Electroosmotic Flow Induced Lift Forces on Polymer Chains in Nanochannels.

A major objective of research in nanofluidics is to achieve better selectivity in manipulating the fluxes of nano-objects and in particular of biopolymers. Numerical simulations allow one to better understand the physical mechanisms at play in such situations. We performed hybrid mesoscale simulations to investigate the properties of polymers under flows in slit pores at the nanoscale. We use multiparticle collision dynamics, an algorithm that includes hydrodynamics and thermal fluctuations, to investigate the properties of fully flexible and stiff polymers under several types of flow, showing that Poiseuille flows and electroosmotic flows can lead to quantitatively and qualitatively different behaviors of the chain. In particular, a counterintuitive phenomenon occurs in the presence of an electroosmotic flow: When the monomers are attracted by the solid surfaces through van der Waals forces, shear-induced forces lead to a stronger repulsion of the polymers from these surfaces. Such focusing of the chain in the middle of the channel increases its flowing velocity, a phenomenon that may be exploited to separate different types of polymers.

Emergence of active turbulence in microswimmer suspensions due to active hydrodynamic stress and volume exclusion

Microswimmers exhibit an intriguing, highly-dynamic collective motion with large-scale swirling and streaming patterns, denoted as active turbulence – reminiscent of classical high-Reynolds-number hydrodynamic turbulence. Various experimental, numerical, and theoretical approaches have been applied to elucidate similarities and differences of inertial hydrodynamic and active turbulence. We use squirmers embedded in a mesoscale fluid, modeled by the multiparticle collision dynamics (MPC) approach, to explore the collective behavior of bacteria-type microswimmers. Our model includes the active hydrodynamic stress generated by propulsion, and a rotlet dipole characteristic for flagellated bacteria. We find emergent clusters, activity-induced phase separation, and swarming behavior, depending on density, active stress, and the rotlet dipole strength. The analysis of the squirmer dynamics in the swarming phase yields Kolomogorov-Kraichnan-type hydrodynamic turbulence and energy spectra for sufficiently high concentrations and a strong rotlet dipole. This emphasizes the paramount importance of the hydrodynamic flow field for swarming motility and bacterial turbulence.