Clustering of self-thermophilic asymmetric dimers: the relevance of hydrodynamics.

Self-thermophilic dimers are characterized by a net phoretic attraction which, in combination with hydrodynamic interactions, results in the formation of crystalline-like aggregates. To distinguish the effect of the different contributions is frequently an important challenge. We present a simulation investigation done in parallel in the presence and the absence of hydrodynamic interactions for the case of asymmetric self-thermophoretic dimers. In the absence of hydrodynamics, the clusters have the standard heads-in configurations. In contrast, in the presence of hydrodynamics, clusters with heads-in conformation are being formed, in which dimers with their propulsion velocity pointing out of the cluster are assembled and stabilized by strong hydrodynamic osmotic flows. Significant variation in the material properties is to be expected from such differences in the collective behavior, whose understanding and control is of great relevance for the development of new synthetic active materials.

Self-phoretic Brownian dynamics simulations.

A realistic and effective model to simulate phoretic Brownian dynamics swimmers based on the general form of the thermophoretic force is here presented. The collective behavior of self-phoretic dimers is investigated with this model and compared with two simpler versions, allowing the understanding of the subtle interplay of steric interactions, propulsion, and phoretic effects. The phoretic Brownian dynamics method has control parameters which can be tuned to closely map the properties of experiments or simulations with explicit solvent, in particular those performed with multiparticle collision dynamics. The combination of the phoretic Brownian method and multiparticle collision dynamics is a powerful tool to precisely identify the importance of hydrodynamic interactions in systems of self-phoretic swimmers.

Collective behavior of thermophoretic dimeric active colloids in three-dimensional bulk.

Colloids driven by phoresis constitute one of the main avenues for the design of synthetic microswimmers. For these swimmers, the specific form of the phoretic and hydrodynamic interactions dramatically influences their dynamics. Explicit solvent simulations allow the investigation of the different behaviors of dimeric Janus active colloids. The phoretic character is modified from thermophilic to thermophobic, and this, together with the relative size of the beads, strongly influences the resulting solvent velocity fields. Hydrodynamic flows can change from puller-type to pusher-type, although the actual flows significantly differ from these standard flows. Such hydrodynamic interactions combined with phoretic interactions between dimers result in several interesting phenomena in three-dimensional bulk conditions. Thermophilic dimeric swimmers are attracted to each other and form large and stable aggregates. Repulsive phoretic interactions among thermophobic dimeric swimmers hinder such clustering and lead, together with long- and short-ranged attractive hydrodynamic interactions, to short-lived, aligned swarming structures.

Filamentous active matter: Band formation, bending, buckling, and defects.

Motor proteins drive persistent motion and self-organization of cytoskeletal filaments. However, state-of-the-art microscopy techniques and continuum modeling approaches focus on large length and time scales. Here, we perform component-based computer simulations of polar filaments and molecular motors linking microscopic interactions and activity to self-organization and dynamics from the filament level up to the mesoscopic domain level. Dynamic filament cross-linking and sliding and excluded-volume interactions promote formation of bundles at small densities and of active polar nematics at high densities. A buckling-type instability sets the size of polar domains and the density of topological defects. We predict a universal scaling of the active diffusion coefficient and the domain size with activity, and its dependence on parameters like motor concentration and filament persistence length. Our results provide a microscopic understanding of cytoplasmic streaming in cells and help to develop design strategies for novel engineered active materials.

The 2020 motile active matter roadmap.

Activity and autonomous motion are fundamental in living and engineering systems. This has stimulated the new field of 'active matter' in recent years, which focuses on the physical aspects of propulsion mechanisms, and on motility-induced emergent collective behavior of a larger number of identical agents. The scale of agents ranges from nanomotors and microswimmers, to cells, fish, birds, and people. Inspired by biological microswimmers, various designs of autonomous synthetic nano- and micromachines have been proposed. Such machines provide the basis for multifunctional, highly responsive, intelligent (artificial) active materials, which exhibit emergent behavior and the ability to perform tasks in response to external stimuli. A major challenge for understanding and designing active matter is their inherent nonequilibrium nature due to persistent energy consumption, which invalidates equilibrium concepts such as free energy, detailed balance, and time-reversal symmetry. Unraveling, predicting, and controlling the behavior of active matter is a truly interdisciplinary endeavor at the interface of biology, chemistry, ecology, engineering, mathematics, and physics. The vast complexity of phenomena and mechanisms involved in the self-organization and dynamics of motile active matter comprises a major challenge. Hence, to advance, and eventually reach a comprehensive understanding, this important research area requires a concerted, synergetic approach of the various disciplines. The 2020 motile active matter roadmap of Journal of Physics: Condensed Matter addresses the current state of the art of the field and provides guidance for both students as well as established scientists in their efforts to advance this fascinating area.

Dissipative particle dynamics with energy conservation: Isoenergetic integration and transport properties.

Simulations of nano- to micro-meter scale fluidic systems under thermal gradients require consistent mesoscopic methods accounting for both hydrodynamic interactions and proper transport of energy. One such method is dissipative particle dynamics with energy conservation (DPDE), which has been used for various fluid systems with non-uniform temperature distributions. We propose an easily parallelizable modification of the velocity-Verlet algorithm based on local energy redistribution for each DPDE particle such that the total energy in a simulated system is conserved up to machine precision. Furthermore, transport properties of a DPDE fluid are analyzed in detail. In particular, an analytical approximation for the thermal conductivity coefficient is derived, which allows its a priori estimation for a given parameter set. Finally, we provide approximate expressions for the dimensionless Prandtl and Schmidt numbers, which characterize fluid transport properties and can be adjusted independently by a proper selection of model parameters. In conclusion, our results strengthen the DPDE method as a very robust approach for the investigation of mesoscopic systems with temperature inhomogeneities.

Tumbling of Quantum Dots: Rheo-Optics.

Linear flow dichroism is shown to be a powerful tool to characterize the hydrodynamic dimensions of extremely small nonspherical colloids in solution. Dispersions of prolate and oblate quantum dots (QDs) are employed to investigate the validity of flow dichroism as a characterization tool. Shape-anisotropic QDs are important from an application perspective, where it is necessary to have a good knowledge of their hydrodynamic dimensions to predict and control their orientation during solution processing. Flow dichroism quantifies the tumbling motion of QDs in shear flow by optical means, which provides a characteristic signature of the particle shape, hydrodynamic friction, and size distribution. The effects of particle size and shape, size polydispersity, and shear rate on the temporal evolution of the flow-induced alignment are discussed in detail on the basis of numerical solutions of the Smoluchowski equation that describes the motion for the probability of the orientation of colloids in shear flow. It is shown that the combination of flow-dichroism experiments and the theoretical approach on the basis of the Smoluchowski equation provides a means to measure hydrodynamic aspect ratios and polydispersity, which for such small particles is not feasible with standard methods similar to light scattering. Flow dichroism will be useful not only for shape-anisotropic colloidal QDs, but also for other nanoscale systems.

Trefoil Knot Hydrodynamic Delocalization on Sheared Ring Polymers.

The behavior of unknotted and trefoil-knotted ring polymers under shear flow is here examined by means of mesoscopic simulations. In contrast to most polymers, ring polymers in a hydrodynamic solvent at high shear rates do not get shortened in the vorticity direction. This is a consequence of the backflow produced by the interaction of the sheared solvent with the end-free polymer topology. The extended structures of the ring in the vorticity-flow plane, when they are aligned in a constant velocity plane, favor ring contour fluctuations. This variety of conformations largely suppresses the tank-treading type of rotation with extended conformations in favor of the tumbling type of rotations, where stretched and collapsed conformations alternate. The extension of trefoil knots is also enhanced, so that the knots become delocalized. We anticipate that these effects, which disappear in the absence of hydrodynamic interactions, will have a crucial impact on the rheological properties of concentrated ring solutions, and will also influence the behavior of more complicated systems such as mixtures of polymers with different topologies.

Anisotropic thermophoresis.

Colloidal migration in a temperature gradient is referred to as thermophoresis. In contrast to particles with a spherical shape, we show that elongated colloids may have a thermophoretic response that varies with the colloid orientation. Remarkably, this can translate into a non-vanishing thermophoretic force in the direction perpendicular to the temperature gradient. Opposite to the friction force, the thermophoretic force of a rod oriented with the temperature gradient can be larger or smaller than when oriented perpendicular to it. The precise anisotropic thermophoretic behavior clearly depends on the colloidal rod aspect ratio, and also on its surface details, which provides an interesting tunability to the devices constructed based on this principle. By means of mesoscale hydrodynamic simulations, we characterize this effect for different types of rod-like colloids.

Chemically driven fluid transport in long microchannels.

Chemical gradients maintained along surfaces can drive fluid flows by diffusio-osmosis, which become significant at micro- and nano-scales. Here, by means of mesoscopic simulations, we show that a concentration drop across microchannels with periodically inhomogeneous boundary walls can laterally transport fluids over arbitrarily long distances along the microchannel. The driving field is the secondary local chemical gradient parallel to the channel induced by the periodic inhomogeneity of the channel wall. The flow velocity depends on the concentration drop across the channel and the structure and composition of the channel walls, but it is independent of the overall channel length. Our work thus presents new insight into the fluid transport in long microchannels commonly found in nature and is useful for designing novel micro- or nano-fluidic pumps.

Thermoosmotic microfluidics.

Microchannels with asymmetrically ratcheted walls are here shown to behave as effective and versatile microfluidic pumps if locally heated. When the boundary walls have different temperatures, the confined liquid experiences a temperature gradient along the sawtooth edges, which can induce a thermoosmotic flow. A mesoscale molecular simulation approach is here employed to investigate the flows which are contrasted using an analytical approach. Microchannels can be composed by one or two ratcheted walls which can be straight or cylindrical. Varying the channel geometry can not only change the overall fluid flux, but also vary the flow patters from shear to capillary type, or even to extensional type flows. This scheme does not require multiphase fluids or any movable channel parts, although they are possible to be implemented. The proposed principle is then very versatile to locally manipulate complex fluids, and a promising tool to recover waste heat, to facilitate cooling of microchips, and to manufacture portable lab-on-a-chip devices.

Effect of angular momentum conservation on hydrodynamic simulations of colloids.

In contrast to most real fluids, angular momentum is not a locally conserved quantity in some mesoscopic simulation methods. Here we quantify the importance of this conservation in the flow fields associated with different colloidal systems. The flow field is analytically calculated with and without angular momentum conservation for the multiparticle collision dynamics (MPC) method, and simulations are performed to verify the predictions. The flow field generated around a colloidal particle moving under an external force with slip boundary conditions depends on the conservation of angular momentum, and the amplitude of the friction force is substantially affected. Interestingly, no dependence on the angular momentum conservation is found for the flow fields generated around colloids under the influence of phoretic forces. Moreover, circular Couette flow between a no-slip and a slip cylinder is investigated, which allows us to validate one of the two existing expressions for the MPC stress tensor.

Trains, tails and loops of partially adsorbed semi-flexible filaments.

Polymer adsorption is a fundamental problem in statistical mechanics that has direct relevance to diverse disciplines ranging from biological lubrication to stability of colloidal suspensions. We combine experiments with computer simulations to investigate depletion induced adsorption of semi-flexible polymers onto a hard-wall. Three dimensional filament configurations of partially adsorbed F-actin polymers are visualized with total internal reflection fluorescence microscopy. This information is used to determine the location of the adsorption/desorption transition and extract the statistics of trains, tails and loops of partially adsorbed filament configurations. In contrast to long flexible filaments which primarily desorb by the formation of loops, the desorption of stiff, finite-sized filaments is largely driven by fluctuating filament tails. Simulations quantitatively reproduce our experimental data and allow us to extract universal laws that explain scaling of the adsorption-desorption transition with relevant microscopic parameters. Our results demonstrate how the adhesion strength, filament stiffness, length, as well as the configurational space accessible to the desorbed filament can be used to design the characteristics of filament adsorption and thus engineer properties of composite biopolymeric materials.

A microscale turbine driven by diffusive mass flux.

An external diffusive mass flux is shown to be able to generate a mechanical torque on a microscale object based on anisotropic diffusiophoresis. In light of this finding, we propose a theoretical prototype micro-turbine driven purely by diffusive mass flux, which is in strong contrast to conventional turbines driven by convective mass flows. The rotational velocity of the proposed turbine is determined by the external concentration gradient, the geometry and the diffusiophoretic properties of the turbine. This scenario is validated by performing computer simulations. Our finding thus provides a new type of chemo-mechanical response which could be used to exploit existing chemical energies at small scales.

Catalytic microrotor driven by geometrical asymmetry.

An asymmetric gear with homogeneous surface properties is, here, presented as a prototype to fabricate catalytic microrotors. The driving torque arises from the diffusiophoretic effect induced by the concentration gradients generated by catalytic chemical reactions at the gear surface. This torque produces a spontaneous and unidirectional rotation of the asymmetric gear. By means of mesoscopic simulations, we prove and characterize this scenario. The gear rotational velocity is determined by the gear-solvent interactions, the gear geometry, the solvent viscosity, and the catalytic reaction ratio. Our work presents a simple way to design self-propelled microrotors, alternative to existing catalytic bi-component, or thermophoretic ones.

A microscale thermophoretic turbine driven by external diffusive heat flux.

We propose a theoretical prototype of a micro-scale turbine externally driven by diffusive heat flux without the need for macroscopic particle flux, which is in sharp contrast to conventional turbines. The prototypes are described analytically and validated by computer simulations. Our results indicate that a micro-scale turbine composed of anisotropic blades can rotate unidirectionally in an external temperature gradient due to the anisotropic thermophoresis effect. The rotational direction and speed depend on the temperature gradient, the geometry and the thermophoretic properties of the turbine. The proposed thermophoretic turbines can be experimentally realized and implemented on micro-devices such as computer-chips to recover waste heat or to facilitate cooling.

Hydrodynamic simulations of self-phoretic microswimmers.

A mesoscopic hydrodynamic model to simulate synthetic self-propelled Janus particles which is thermophoretically or diffusiophoretically driven is here developed. We first propose a model for a passive colloidal sphere which reproduces the correct rotational dynamics together with strong phoretic effect. This colloid solution model employs a multiparticle collision dynamics description of the solvent, and combines stick boundary conditions with colloid-solvent potential interactions. Asymmetric and specific colloidal surface is introduced to produce the properties of self-phoretic Janus particles. A comparative study of Janus and microdimer phoretic swimmers is performed in terms of their swimming velocities and induced flow behavior. Self-phoretic microdimers display long range hydrodynamic interactions with a decay of 1/r(2), which is similar to the decay of gradient fields generated by self-phoretic particle, and can be characterized as pullers or pushers. In contrast, Janus particles are characterized by short range hydrodynamic interactions with a decay of 1/r(3) and behave as neutral swimmers.

A self-propelled thermophoretic microgear.

An asymmetric microgear will spontaneously and unidirectionally rotate if it is heated in a cool surrounding solvent. The resulting temperature gradient along the edges of the gear teeth translates in a directed thermophoretic force, which will exert a net torque on the gear. By means of computer simulations, the validity of this scenario is proved. The rotational direction and speed are dependent on gear­solvent interactions, and can be analytically related to system parameters like the thermal diffusion factor, the solvent viscosity, or the temperature difference. This microgear provides a simple way to extract net work from non-isothermal solutions, and can become a valuable tool in microfluids.

Brownian motion in inhomogeneous suspensions.

The Langevin description of Brownian motion in inhomogeneous suspensions is here revisited. Inhomogeneous suspensions are characterized by a position-dependent friction coefficient, which can significantly influence the dynamics of the suspended particles. Outstanding examples are suspensions in confinement or in the presence of a temperature gradient. The Langevin approach in inhomogeneous systems encounters a fundamental difficulty related to the interpretation of the multiplicative noise induced by the position-dependent friction. We show that the so-called Ito-Stratonovich dilemma is originated by the violation of the macroscopic force balance condition in the traditional procedure of eliminating the fast variables. Repairing this deficit, we rederive the extended overdamped Langevin equation directly from the infradamped Langevin equation. This is without invoking the Fokker-Planck formalism, such that the self-completeness of the Langevin framework is restored. Furthermore, we derive the generalized forms of the drift-force relation and the Smoluchowski equation for inhomogeneous suspensions in a straightforward manner.

Collective thermodiffusion of colloidal suspensions.

The thermophoretic behavior of concentrated colloidal suspensions can be understood as the sum of single particle and collective effects. Here, we present a simulation model to investigate the particularities of the collective thermodiffusive effects in concentrated uncharged solutions, where the influence of different colloid-colloid interactions is analyzed. The concentration dependence found in our simulations qualitatively agrees with experimental results. Colloids with repulsive interactions are found to accumulate more effectively than the solvent in the warm areas, such that the corresponding Soret coefficients are negative and decrease with increasing concentration. The accumulation of colloids in the cold regions is facilitated by attraction, such that colloids with attractive interactions have larger values of the Soret coefficient. A thermodynamic argument that explains our results from equilibrium quantities is discussed as well.