Near-field hydrodynamic interactions determine travelling wave directions of collectively beating cilia.

Cilia can beat collectively in the form of a metachronal wave, and we investigate how near-field hydrodynamic interactions between cilia can influence the collective response of the beating cilia. Based on the theoretical framework developed in the work of Meng et al. (Meng et al. 2021 Proc. Natl Acad. Sci. USA 118, e2102828118), we find that the first harmonic mode in the driving force acting on each individual cilium can determine the direction of the metachronal wave after considering the finite size of the beating trajectories, which is confirmed by our agent-based numerical simulations. The stable wave patterns, e.g. the travelling direction, can be controlled by the driving forces acting on the cilia, based on which one can change the flow field generated by the cilia. This work can not only help to understand the role of the hydrodynamic interactions in the collective behaviours of cilia, but can also guide future designs of artificial cilia beating in the desired dynamic mode.

Molecular dynamics simulations of microscopic structural transition and macroscopic mechanical properties of magnetic gels.

Magnetic gels with embedded micro-/nano-sized magnetic particles in cross-linked polymer networks can be actuated by external magnetic fields, with changes in their internal microscopic structures and macroscopic mechanical properties. We investigate the responses of such magnetic gels to an external magnetic field, by means of coarse-grained molecular dynamics simulations. We find that the dynamics of magnetic particles are determined by the interplay of magnetic dipole-dipole interactions, polymer elasticity, and thermal fluctuations. The corresponding microscopic structures formed by the magnetic particles, such as elongated chains, can be controlled by the external magnetic field. Furthermore, the magnetic gels can exhibit reinforced macroscopic mechanical properties, where the elastic modulus increases algebraically with the magnetic moments of the particles in the form of ∝(m-mc)2 when magnetic chains are formed. This simulation work can not only serve as a tool for studying the microscopic and the macroscopic responses of the magnetic gels, but also facilitate future fabrications and practical controls of magnetic composites with desired physical properties.

Scaling Transition of Active Turbulence from Two to Three Dimensions.

Turbulent flows are observed in low-Reynolds active fluids, which display similar phenomenology to the classical inertial turbulence but are of a different nature. Understanding the dependence of this new type of turbulence on dimensionality is a fundamental challenge in non-equilibrium physics. Real-space structures and kinetic energy spectra of bacterial turbulence are experimentally measured from two to three dimensions. The turbulence shows three regimes separated by two critical confinement heights, resulting from the competition of bacterial length, vortex size and confinement height. Meanwhile, the kinetic energy spectra display distinct universal scaling laws in quasi-2D and 3D regimes, independent of bacterial activity, length, and confinement height, whereas scaling exponents transition in two steps around the critical heights. The scaling behaviors are well captured by the hydrodynamic model we develop, which employs image systems to represent the effects of confining boundaries. The study suggests a framework for investigating the effect of dimensionality on non-equilibrium self-organized systems.

Anomalous Fluctuations in a Droplet of Chemically Active Colloids or Enzymes.

Chemically active colloids or enzymes cluster into dense droplets driven by their phoretic response to collectively generated chemical gradients. Employing Brownian dynamics simulation techniques, our study of the dynamics of such a chemically active droplet uncovers a rich variety of structures and dynamical properties, including the full range of fluidlike to solidlike behavior, and non-Gaussian positional fluctuations. Our work sheds light on the complex dynamics of the active constituents of metabolic clusters, which are the main drivers of nonequilibrium activity in living systems.

Escaping Kinetic Traps Using Nonreciprocal Interactions.

Kinetic traps are a notorious problem in equilibrium statistical mechanics, where temperature quenches ultimately fail to bring the system to low energy configurations. Using multifarious self-assembly as a model system, we introduce a mechanism to escape kinetic traps by utilizing nonreciprocal interactions between components. Introducing nonequilibrium effects offered by broken action-reaction symmetry in the system pushes the trajectory of the system out of arrested dynamics. The dynamics of the model is studied using tools from the physics of interfaces and defects. Our proposal can find applications in self-assembly, glassy systems, and systems with arrested dynamics to facilitate escape from local minima in rough energy landscapes.

Nanocrystal Assemblies: Current Advances and Open Problems.

We explore the potential of nanocrystals (a term used equivalently to nanoparticles) as building blocks for nanomaterials, and the current advances and open challenges for fundamental science developments and applications. Nanocrystal assemblies are inherently multiscale, and the generation of revolutionary material properties requires a precise understanding of the relationship between structure and function, the former being determined by classical effects and the latter often by quantum effects. With an emphasis on theory and computation, we discuss challenges that hamper current assembly strategies and to what extent nanocrystal assemblies represent thermodynamic equilibrium or kinetically trapped metastable states. We also examine dynamic effects and optimization of assembly protocols. Finally, we discuss promising material functions and examples of their realization with nanocrystal assemblies.

Chemotactic particles as strong electrolytes: Debye-Hückel approximation and effective mobility law.

We consider a binary mixture of chemically active particles that produce or consume solute molecules and that interact with each other through the long-range concentration fields they generate. We analytically calculate the effective phoretic mobility of these particles when the mixture is submitted to a constant, external concentration gradient, at leading order in the overall concentration. Relying on an analogy with the modeling of strong electrolytes, we show that the effective phoretic mobility decays with the square root of the concentration: our result is, therefore, a nonequilibrium counterpart to the celebrated Kohlrausch and Debye-Hückel-Onsager conductivity laws for electrolytes, which are extended here to particles with long-range nonreciprocal interactions. The effective mobility law we derive reveals the existence of a regime of maximal mobility and could find applications in the description of nanoscale transport phenomena in living cells.

Scale-Dependent Heat Transport in Dissipative Media via Electromagnetic Fluctuations.

We develop a theory for heat transport via electromagnetic waves inside media, and use it to derive a spatially nonlocal thermal conductivity tensor, in terms of the electromagnetic Green's function and potential, for any given system. While typically negligible for optically dense bulk media, the electromagnetic component of conductivity can be significant for optically dilute media, and shows regimes of Fourier transport as well as unhindered transport. Moreover, the electromagnetic contribution is relevant even for dense media, when in the presence of interfaces, as exemplified for the in-plane conductivity of a nanosheet, which shows a variety of phenomena, including absence of a Fourier regime.

A DNA turbine powered by a transmembrane potential across a nanopore.

Rotary motors play key roles in energy transduction, from macroscale windmills to nanoscale turbines such as ATP synthase in cells. Despite our abilities to construct engines at many scales, developing functional synthetic turbines at the nanoscale has remained challenging. Here, we experimentally demonstrate rationally designed nanoscale DNA origami turbines with three chiral blades. These DNA nanoturbines are 24-27 nm in height and diameter and can utilize transmembrane electrochemical potentials across nanopores to drive DNA bundles into sustained unidirectional rotations of up to 10 revolutions s-1. The rotation direction is set by the designed chirality of the turbine. All-atom molecular dynamics simulations show how hydrodynamic flows drive this turbine. At high salt concentrations, the rotation direction of turbines with the same chirality is reversed, which is explained by a change in the anisotropy of the electrophoretic mobility. Our artificial turbines operate autonomously in physiological conditions, converting energy from naturally abundant electrochemical potentials into mechanical work. The results open new possibilities for engineering active robotics at the nanoscale.

Enhanced diffusion of tracer particles in nonreciprocal mixtures.

We study the diffusivity of a tagged particle in a binary mixture of Brownian particles with nonreciprocal interactions. Numerical simulations reveal that, for a broad class of interaction potentials, nonreciprocity can significantly increase the long-time diffusion coefficient of tracer particles and that this diffusion enhancement is associated with a breakdown of the Einstein relation. These observations are quantified and confirmed via two different and complementary analytical approaches: (i) a linearized stochastic density field theory, which is particularly accurate in the limit of soft interactions, and (ii) a reduced two-body description, which is exact at leading order in the density of particles. The latter reveals that diffusion enhancement can be attributed to the formation of transiently propelled dimers of particles, whose cohesion and speed are controlled by the nonreciprocal interactions.

Lorentz Reciprocal Theorem in Fluids with Odd Viscosity.

The Lorentz reciprocal theorem-that is used to study various transport phenomena in hydrodynamics-is violated in chiral active fluids that feature odd viscosity with broken time-reversal and parity symmetries. Here, we show that the theorem can be generalized to fluids with odd viscosity by choosing an auxiliary problem with the opposite sign of the odd viscosity. We demonstrate the application of the theorem to two categories of microswimmers. Swimmers with prescribed surface velocity are not affected by odd viscosity, while those with prescribed active forces are. In particular, a torque dipole can lead to directed motion.

Dynamical Pattern Formation without Self-Attraction in Quorum-Sensing Active Matter: The Interplay between Nonreciprocity and Motility.

We study a minimal model involving two species of particles interacting via quorum-sensing rules. Combining simulations of the microscopic model and linear stability analysis of the associated coarse-grained field theory, we identify a mechanism for dynamical pattern formation that does not rely on the standard route of intraspecies effective attractive interactions. Instead, our results reveal a highly dynamical phase of chasing bands induced only by the combined effects of self-propulsion and nonreciprocity in the interspecies couplings. Turning on self-attraction, we find that the system may phase separate into a macroscopic domain of such chaotic chasing bands coexisting with a dilute gas. We show that the chaotic dynamics of bands at the interfaces of this phase-separated phase results in anomalously slow coarsening.

Network Effects Lead to Self-Organization in Metabolic Cycles of Self-Repelling Catalysts.

Mixtures of particles that interact through phoretic effects are known to aggregate if they belong to species that exhibit attractive self-interactions. We study self-organization in a model metabolic cycle composed of three species of catalytically active particles that are chemotactic toward the chemicals that define their connectivity network. We find that the self-organization can be controlled by the network properties, as exemplified by a case where a collapse instability is achieved by design for self-repelling species. Our findings highlight a possibility for controlling the intricate functions of metabolic networks by taking advantage of the physics of phoretic active matter.

Nonreciprocal interactions give rise to fast cilium synchronization in finite systems.

Motile cilia beat in an asymmetric fashion in order to propel the surrounding fluid. When many cilia are located on a surface, their beating can synchronize such that their phases form metachronal waves. Here, we computationally study a model where each cilium is represented as a spherical particle, moving along a tilted trajectory with a position-dependent active driving force and a position-dependent internal drag coefficient. The model thus takes into account all the essential broken symmetries of the ciliary beat. We show that taking into account the near-field hydrodynamic interactions, the effective coupling between cilia even over an entire beating cycle can become nonreciprocal: The phase of a cilium is more strongly affected by an adjacent cilium on one side than by a cilium at the same distance in the opposite direction. As a result, synchronization starts from a seed at the edge of a group of cilia and propagates rapidly across the system, leading to a synchronization time that scales proportionally to the linear dimension of the system. We show that a ciliary carpet is characterized by three different velocities: the velocity of fluid transport, the phase velocity of metachronal waves, and the group velocity of order propagation. Unlike in systems with reciprocal coupling, boundary effects are not detrimental for synchronization, but rather enable the formation of the initial seed.

Minimum entropy production by microswimmers with internal dissipation.

The energy dissipation and entropy production by self-propelled microswimmers differ profoundly from passive particles pulled by external forces. The difference extends both to the shape of the flow around the swimmer, as well as to the internal dissipation of the propulsion mechanism. Here we derive a general theorem that provides an exact lower bound on the total, external and internal, dissipation by a microswimmer. The problems that can be solved include an active surface-propelled droplet, swimmers with an extended propulsive layer and swimmers with an effective internal dissipation. We apply the theorem to determine the swimmer shapes that minimize the total dissipation while keeping the volume constant. Our results show that the entropy production by active microswimmers is subject to different fundamental limits than the entropy production by externally driven particles.

Self-organization of primitive metabolic cycles due to non-reciprocal interactions.

One of the greatest mysteries concerning the origin of life is how it has emerged so quickly after the formation of the earth. In particular, it is not understood how metabolic cycles, which power the non-equilibrium activity of cells, have come into existence in the first instances. While it is generally expected that non-equilibrium conditions would have been necessary for the formation of primitive metabolic structures, the focus has so far been on externally imposed non-equilibrium conditions, such as temperature or proton gradients. Here, we propose an alternative paradigm in which naturally occurring non-reciprocal interactions between catalysts that can partner together in a cyclic reaction lead to their recruitment into self-organized functional structures. We uncover different classes of self-organized cycles that form through exponentially rapid coarsening processes, depending on the parity of the cycle and the nature of the interaction motifs, which are all generic but have readily tuneable features.

Pair Interaction between Two Catalytically Active Colloids.

Due to the intrinsically complex non-equilibrium behavior of the constituents of active matter systems, a comprehensive understanding of their collective properties is a challenge that requires systematic bottom-up characterization of the individual components and their interactions. For self-propelled particles, intrinsic complexity stems from the fact that the polar nature of the colloids necessitates that the interactions depend on positions and orientations of the particles, leading to a 2d - 1 dimensional configuration space for each particle, in d dimensions. Moreover, the interactions between such non-equilibrium colloids are generically non-reciprocal, which makes the characterization even more complex. Therefore, derivation of generic rules that enable us to predict the outcomes of individual encounters as well as the ensuing collective behavior will be an important step forward. While significant advances have been made on the theoretical front, such systematic experimental characterizations using simple artificial systems with measurable parameters are scarce. Here, two different contrasting types of colloidal microswimmers are studied, which move in opposite directions and show distinctly different interactions. To facilitate the extraction of parameters, an experimental platform is introduced in which these parameters are confined on a 1D track. Furthermore, a theoretical model for interparticle interactions near a substrate is developed, including both phoretic and hydrodynamic effects, which reproduces their behavior. For subsequent validation, the degrees of freedom are increased to 2D motion and resulting trajectories are predicted, finding remarkable agreement. These results may prove useful in characterizing the overall alignment behavior of interacting self-propelling active swimmer and may find direct applications in guiding the design of active-matter systems involving phoretic and hydrodynamic interactions.

Steering self-organisation through confinement.

Self-organisation is the spontaneous emergence of spatio-temporal structures and patterns from the interaction of smaller individual units. Examples are found across many scales in very different systems and scientific disciplines, from physics, materials science and robotics to biology, geophysics and astronomy. Recent research has highlighted how self-organisation can be both mediated and controlled by confinement. Confinement is an action over a system that limits its units' translational and rotational degrees of freedom, thus also influencing the system's phase space probability density; it can function as either a catalyst or inhibitor of self-organisation. Confinement can then become a means to actively steer the emergence or suppression of collective phenomena in space and time. Here, to provide a common framework and perspective for future research, we examine the role of confinement in the self-organisation of soft-matter systems and identify overarching scientific challenges that need to be addressed to harness its full scientific and technological potential in soft matter and related fields. By drawing analogies with other disciplines, this framework will accelerate a common deeper understanding of self-organisation and trigger the development of innovative strategies to steer it using confinement, with impact on, e.g., the design of smarter materials, tissue engineering for biomedicine and in guiding active matter.

Non-reciprocal multifarious self-organization.

A hallmark of living systems is the ability to employ a common set of building blocks that can self-organize into a multitude of different structures. This capability can only be afforded in non-equilibrium conditions, as evident from the energy-consuming nature of the plethora of such dynamical processes. To achieve automated dynamical control of such self-assembled structures and transitions between them, we need to identify the fundamental aspects of non-equilibrium dynamics that can enable such processes. Here we identify programmable non-reciprocal interactions as a tool to achieve such functionalities. The design rule is composed of reciprocal interactions that lead to the equilibrium assembly of the different structures, through a process denoted as multifarious self-assembly, and non-reciprocal interactions that give rise to non-equilibrium dynamical transitions between the structures. The design of such self-organized shape-shifting structures can be implemented at different scales, from nucleic acids and peptides to proteins and colloids.