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To impart directionality to the motions of a molecular mechanism, one must overcome the random thermal forces that are ubiquitous on such small scales and in liquid solution at ambient temperature. In equilibrium without energy supply, directional motion cannot be sustained without violating the laws of thermodynamics. Under conditions away from thermodynamic equilibrium, directional motion may be achieved within the framework of Brownian ratchets, which are diffusive mechanisms that have broken inversion symmetry1-5. Ratcheting is thought to underpin the function of many natural biological motors, such as the F1F0-ATPase6-8, and it has been demonstrated experimentally in synthetic microscale systems (for example, to our knowledge, first in ref. 3) and also in artificial molecular motors created by organic chemical synthesis9-12. DNA nanotechnology13 has yielded a variety of nanoscale mechanisms, including pivots, hinges, crank sliders and rotary systems14-17, which can adopt different configurations, for example, triggered by strand-displacement reactions18,19 or by changing environmental parameters such as pH, ionic strength, temperature, external fields and by coupling their motions to those of natural motor proteins20-26. This previous work and considering low-Reynolds-number dynamics and inherent stochasticity27,28 led us to develop a nanoscale rotary motor built from DNA origami that is driven by ratcheting and whose mechanical capabilities approach those of biological motors such as F1F0-ATPase.
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DNA , Difusão Facilitada , Proteínas Motores Moleculares , DNA/química , Concentração de Íons de Hidrogênio , Proteínas Motores Moleculares/química , Proteínas Motores Moleculares/metabolismo , Movimento (Física) , Movimento , Concentração Osmolar , ATPases Translocadoras de Prótons/química , ATPases Translocadoras de Prótons/metabolismo , Processos Estocásticos , Temperatura , TermodinâmicaRESUMO
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.
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A common feature of biological self-organization is how active agents communicate with each other or their environment via chemical signaling. Such communications, mediated by self-generated chemical gradients, have consequences for both individual motility strategies and collective migration patterns. Here, in a purely physicochemical system, we use self-propelling droplets as a model for chemically active particles that modify their environment by leaving chemical footprints, which act as chemorepulsive signals to other droplets. We analyze this communication mechanism quantitatively both on the scale of individual agent-trail collisions as well as on the collective scale where droplets actively remodel their environment while adapting their dynamics to that evolving chemical landscape. We show in experiment and simulation how these interactions cause a transient dynamical arrest in active emulsions where swimmers are caged between each other's trails of secreted chemicals. Our findings provide insight into the collective dynamics of chemically active particles and yield principles for predicting how negative autochemotaxis shapes their navigation strategy.
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Quimiotaxia , Simulação por Computador , EmulsõesRESUMO
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.
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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.
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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.
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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 â(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.
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On surfaces with many motile cilia, beats of the individual cilia coordinate to form metachronal waves. We present a theoretical framework that connects the dynamics of an individual cilium to the collective dynamics of a ciliary carpet via systematic coarse graining. We uncover the criteria that control the selection of frequency and wave vector of stable metachronal waves of the cilia and examine how they depend on the geometric and dynamical characteristics of a single cilium, as well as the geometric properties of the array. We perform agent-based numerical simulations of arrays of cilia with hydrodynamic interactions and find quantitative agreement with the predictions of the analytical framework. Our work sheds light on the question of how the collective properties of beating cilia can be determined using information about the individual units and, as such, exemplifies a bottom-up study of a rich active matter system.
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Cílios , Modelos Biológicos , Movimento Celular , Cílios/química , Cílios/fisiologia , HidrodinâmicaRESUMO
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.
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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.
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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.
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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.
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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.
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Many functional units in biology, such as enzymes or molecular motors, are composed of several subunits that can reversibly assemble and disassemble. This includes oligomeric proteins composed of several smaller monomers, as well as protein complexes assembled from a few proteins. By studying the generic spatial transport properties of such proteins, we investigate here whether their ability to reversibly associate and dissociate may confer on them a functional advantage with respect to nondissociating proteins. In uniform environments with position-independent association-dissociation, we find that enhanced diffusion in the monomeric state coupled to reassociation into the functional oligomeric form leads to enhanced reactivity with localized targets. In nonuniform environments with position-dependent association-dissociation, caused by, for example, spatial gradients of an inhibiting chemical, we find that dissociating proteins generically tend to accumulate in regions where they are most stable, a process that we term "stabilitaxis."
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Transtornos Dissociativos/metabolismo , Complexos Multiproteicos/química , Proteínas , Microambiente Celular , Difusão , Modelos Teóricos , Complexos Multiproteicos/metabolismo , Polimerização , Estabilidade Proteica , Transporte Proteico , Proteínas/química , Proteínas/metabolismoRESUMO
In their Comment (DOI: 10.1021/jacs.2c02965) on two related publications by our group (J. Am. Chem. Soc. 2022, 144, 1380-1388; DOI: 10.1021/jacs.1c11754) and another (J. Am. Chem. Soc. 2021, 143, 20884-20890; DOI: 10.1021/jacs.1c09455), Huang and Granick refer to the diffusion NMR measurements of molecules during a copper-catalyzed azide-alkyne cycloaddition (CuAAC) "click" reaction. Here we respond to their comments and maintain that no measurable diffusion enhancement was observed during the reaction. We expand on the physical arguments presented in our original JACS Article regarding the appropriate reference state for the diffusion coefficient and present new data showing that the use of other reference states, as suggested by Huang and Granick, will still support our conclusion that the two reactants and one product of the CuAAC reaction do not exhibit boosted mobility during the reaction.
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Azidas , Química Click , Alcinos/química , Azidas/química , Catálise , Cobre/química , Reação de CicloadiçãoRESUMO
Micrometer-sized objects are widely known to exhibit chemically driven motility in systems away from equilibrium. Experimental observation of reaction-induced motility or enhancement in diffusivity at the much shorter length scale of small molecules is, however, still a matter of debate. Here, we investigate the molecular diffusivity of reactants, catalyst, and product of a model reaction, the copper-catalyzed azide-alkyne cycloaddition click reaction, and develop new NMR diffusion approaches that allow the probing of reaction-induced diffusion enhancement in nanosized molecular systems with higher accuracy than the state of the art. Following two different approaches that enable the accounting of time-dependent concentration changes during NMR experiments, we closely monitored the diffusion coefficient of reaction components during the reaction. The reaction components showed distinct changes in the diffusivity: while the two reactants underwent a time-dependent decrease in their diffusivity, the diffusion coefficient of the product gradually increased and the catalyst showed only slight diffusion enhancement within the range expected for reaction-induced sample heating. The decrease in diffusion coefficient of the alkyne, one of the two reactants of click reaction, was not reproduced during its copper coordination when the second reactant, azide, was absent. Our results do not support the catalysis-induced diffusion enhancement of the components of the click reaction and, instead, point to the role of a relatively large intermediate species within the reaction cycle with diffusivity lower than that of both the reactants and product molecule.
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Cilia and flagella are beating rod-like organelles that enable the directional movement of microorganisms in fluids and fluid transport along the surface of biological organisms or inside organs. The molecular motor axonemal dynein drives their beating by interacting with microtubules. Constructing synthetic beating systems with axonemal dynein capable of mimicking ciliary beating still represents a major challenge. Here, the bottom-up engineering of a sustained beating synthoneme consisting of a pair of microtubules connected by a series of periodic arrays of approximately eight axonemal dyneins is reported. A model leads to the understanding of the motion through the cooperative, cyclic association-dissociation of the molecular motor from the microtubules. The synthoneme represents a bottom-up self-organized bio-molecular machine at the nanoscale with cilia-like properties.
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Dineínas do Axonema , Axonema , Dineínas do Axonema/metabolismo , Axonema/metabolismo , Cílios/metabolismo , Dineínas/metabolismo , Flagelos/metabolismo , Microtúbulos/metabolismoRESUMO
We present a thermodynamically consistent model describing the dynamics of a multicomponent mixture where one enzyme component catalyzes a reaction between other components. We find that the catalytic activity alone can induce phase separation for sufficiently active systems and large enzymes, without any equilibrium interactions between components. In the limit of fast reaction rates, binodal lines can be calculated using a mapping to an effective free energy. We also explain how this catalysis-induced phase separation can act to autoregulate the enzymatic activity, which points at the biological relevance of this phenomenon.
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Catálise , HomeostaseRESUMO
We study the dynamics and conformations of a single active semiflexible polymer whose monomers experience a propulsion force perpendicular to the local tangent, with the end beads being different from the inner beads ("end-tailored"). Using Langevin simulations, we demonstrate that, apart from sideways motion, the relative propulsion strength between the end beads and the polymer backbone significantly changes the conformational properties of the polymers as a function of bending stiffness, end-tailoring and propulsion force. Expectedly, for slower ends the polymer curves away from the moving direction, while faster ends lead to opposite curving, in both cases slightly reducing the center of mass velocity compared to a straight fiber. Interestingly, for faster end beads there is a rich and dynamic morphology diagram: the polymer ends may get folded together to 2D loops or hairpin-like conformations that rotate due to their asymmetry in shape and periodic flapping motion around a rather straight state during full propulsion is also possible. We rationalize the simulations using scaling and kinematic arguments and present the state diagram of the conformations. Sideways propelled fibers comprise a rather unexplored and versatile class of self-propellers, and their study will open novel ways for designing, e.g. motile actuators or mixers in soft robotics.
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Fenômenos Mecânicos , Polímeros , Conformação MolecularRESUMO
Gels are soft elastic materials made of a three-dimensional cross-linked polymer network and featuring both elastic and dissipative responses under external mechanical stimuli. Here we investigate how such gels mediate the organization of embedded magnetic microparticles when driven by an external field. By constructing a continuum theory, we demonstrate that the collective dynamics of the embedded particles result from the delicate balance between magnetic dipole-dipole interactions, thermal fluctuations and elasticity of the polymer network, verified by our experiments. The proposed model could be extended to other soft magnetic composites in order to predict how the elastic interactions mediate the aggregation of the embedded elements, fostering technological implications for multifunctional hydrogel materials.