Publications by authors named "John F Brady"

Mechanical properties of disordered materials are governed by their underlying free energy landscape. In contrast to external fields, embedding a small fraction of active particles within a disordered material generates nonequilibrium internal fields, which can help to circumvent kinetic barriers and modulate the free energy landscape. In this work, we investigate through computer simulations how the activity of active particles alters the mechanical response of deeply annealed polydisperse colloidal gels.

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Bacteria can swim upstream in a narrow tube and pose a clinical threat of urinary tract infection to patients implanted with catheters. Coatings and structured surfaces have been proposed to repel bacteria, but no such approach thoroughly addresses the contamination problem in catheters. Here, on the basis of the physical mechanism of upstream swimming, we propose a novel geometric design, optimized by an artificial intelligence model.

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Nonequilibrium phase transitions are routinely observed in both natural and synthetic systems. The ubiquity of these transitions highlights the conspicuous absence of a general theory of phase coexistence that is broadly applicable to both nonequilibrium and equilibrium systems. Here, we present a general mechanical theory for phase separation rooted in ideas explored nearly a half-century ago in the study of inhomogeneous fluids.

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In striking contrast to equilibrium systems, inertia can profoundly alter the structure of active systems. Here, we demonstrate that driven systems can exhibit effective equilibrium-like states with increasing particle inertia, despite rigorously violating the fluctuation-dissipation theorem. Increasing inertia progressively eliminates motility-induced phase separation and restores equilibrium crystallization for active Brownian spheres.

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We analyze a dilute suspension of active particles confined between walls and subjected to fields that can modulate particle speed as well as orientation. Generally, the particle distribution is different in the bulk compared to near the walls. In the bulk, particles tend to accumulate in the regions of low speed, but in the presence of an orienting field normal to the walls, particles rotate to align with the field and accumulate in the field direction.

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Control of self-propelled particles is central to the development of many microrobotic technologies, from dynamically reconfigurable materials to advanced lab-on-a-chip systems. However, there are few physical principles by which particle trajectories can be specified and can be used to generate a wide range of behaviors. Within the field of ray optics, a single principle for controlling the trajectory of light─Snell's law─yields an intuitive framework for engineering a broad range of devices, from microscopes to cameras and telescopes.

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In microrheology, the local rheological properties, such as the viscoelasticity of a complex fluid, are inferred from the free or forced motion of embedded colloidal probe particles. Theoretical machinery developed for forced-probe microrheology of colloidal suspensions focused on either constant-force (CF) or constant-velocity (CV) probes, while in experiments, neither the force nor the kinematics of the probe is fixed. More importantly, the constraint of CF or CV introduces a difficulty in the meaningful quantification of the fluctuations of the probe due to a thermodynamic uncertainty relation.

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Passive Brownian particles partition homogeneously between a porous medium and an adjacent fluid reservoir. In contrast, active particles accumulate near boundaries and can therefore preferentially partition into the porous medium. Understanding how active particles interact with and partition into such an environment is important for optimizing particle transport.

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By introducing the notion of a dynamic overlap concentration scale, we identify additional universal features of the mechanical properties of active colloids. We codify these features by recognizing that the characteristic length scale of an active particle's trajectory, the run length, introduces a concentration scale ϕ^{*}. Large-scale simulations of repulsive active Brownian particles (ABPs) confirm that this run-length dependent concentration, the trajectory-space analog of the overlap concentration in polymer solutions, delineates distinct concentration regimes in which interparticle collisions alter particle trajectories.

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We demonstrate that deep learning techniques can be used to predict motility-induced phase separation (MIPS) in suspensions of active Brownian particles (ABPs) by creating a notion of phase at the particle level. Using a fully connected network in conjunction with a graph neural network we use individual particle features to predict to which phase a particle belongs. From this, we are able to compute the fraction of dilute particles to determine if the system is in the homogeneous dilute, dense, or coexistence region.

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We demonstrate that the mechanically defined "isothermal" compressibility behaves as a thermodynamic-like response function for suspensions of active Brownian particles. The compressibility computed from the active pressure-a combination of the collision and unique swim pressures-is capable of predicting the critical point for motility induced phase separation, as expected from the mechanical stability criterion. We relate this mechanical definition to the static structure factor via an active form of the thermodynamic compressibility equation and find the two to be equivalent, as would be the case for equilibrium systems.

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Active Brownian particles (ABPs) distribute non-homogeneously near surfaces, and understanding how this depends on system properties-size, shape, activity level, etc.-is essential for predicting and exploiting the behavior of active matter systems. Active particles accumulate at no-flux surfaces owing to their persistent swimming, which depends on their intrinsic swim speed and reorientation time, and are subject to confinement effects when their run or persistence length is comparable to the characteristic size of the confining geometry.

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In nonequilibrium active matter systems, a spatial variation in activity can lead to a spatial variation in concentration of active particles satisfying, at steady state, the condition nU=const [Schnitzer, Phys. Rev. E 48, 2553 (1993)1063-651X10.

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The unique pressure exerted by active particles-the "swim" pressure-has proven to be a useful quantity in explaining many of the seemingly confounding behaviors of active particles. However, its use has also resulted in some puzzling findings including an extremely negative surface tension between phase separated active particles. Here, we demonstrate that this contradiction stems from the fact that the swim pressure is not a true pressure.

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The rheological properties of active suspensions are studied via microrheology: tracking the motion of a colloidal probe particle in order to measure the viscoelastic response of the embedding material. The passive probe particle with size R is pulled through the suspension by an external force F, which causes it to translate at some speed U. The bath is comprised of a Newtonian solvent with viscosity η and a dilute dispersion of active Brownian particles (ABPs) with size a, characteristic swim speed U, and a reorientation time τ.

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Thermal motion of particles and molecules in liquids underlies many chemical and biological processes. Liquids, especially in biology, are complex due to structure at multiple relevant length scales. While diffusion in homogeneous simple liquids is well understood through the Stokes-Einstein relation, this equation fails completely in describing diffusion in complex media.

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A consensus has emerged that a constraint to rotational or sliding motion of particles in dense suspensions under flow is the genesis of the discontinuous shear thickening (DST) phenomenon. We show that tangential fluid lubrication interactions due to finite-sized asperities on particle surfaces effectively provide these constraints, changing the dynamics of particle motion. By explicitly resolving for the surface roughness of particles, we show that, while smooth particles exhibit continuous shear thickening, purely hydrodynamic interactions in rough particles result in DST.

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In a colloidal suspension at equilibrium, the diffusive motion of a tracer particle due to random thermal fluctuations from the solvent is related to the particle's response to an applied external force, provided this force is weak compared to the thermal restoring forces in the solvent. This is known as the fluctuation-dissipation theorem (FDT) and is expressed via the Stokes-Einstein-Sutherland (SES) relation D = kT/ζ, where D is the particle's self-diffusivity (fluctuation), ζ is the drag on the particle (dissipation), and kT is the thermal Boltzmann energy. Active suspensions are widely studied precisely because they are far from equilibrium-they can generate significant nonthermal internal stresses, which can break the detailed balance and time-reversal symmetry-and thus cannot be assumed to obey the FDT a priori.

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External fields can decidedly alter the free energy landscape of soft materials and can be exploited as a powerful tool for the assembly of targeted nanostructures and colloidal materials. Here, we use computer simulations to demonstrate that nonequilibrium internal fields or forces-forces that are generated by driven components within a system-in the form of active particles can precisely modulate the dynamical free energy landscape of a model soft material, a colloidal gel. Embedding a small fraction of active particles within a gel can provide a unique pathway for the dynamically frustrated network to circumvent the kinetic barriers associated with reaching a lower free energy state through thermal fluctuations alone.

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We study the motion of a spherical active Brownian particle (ABP) of size a, moving with a fixed speed U0, and reorienting on a time scale τR in the presence of a confining boundary. Because momentum is conserved in the embedding fluid, we show that the average force per unit area on the boundary equals the bulk mechanical pressure P∞ = p∞f + Π∞, where p∞f is the fluid pressure and Π∞ is the particle pressure; this is true for active and passive particles alike regardless of how the particles interact with the boundary. As an example, we investigate how hydrodynamic interactions (HI) change the particle-phase pressure at the wall, and find that Πwall = n∞(kBT + ζ(Δ)U0l(Δ)/6), where ζ is the (Stokes) drag on the swimmer, l = U0τR is the run length, and Δ is the minimum gap size between the particle and the wall; as Δ → ∞ this is the familiar swim pressure [Takatori et al.

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Suspensions of motile bacteria or synthetic microswimmers, termed active matter, manifest a remarkable propensity for self-organization, and formation of large-scale coherent structures. Most active matter research deals with almost homogeneous in space systems and little is known about the dynamics of strongly heterogeneous active matter. Here we report on experimental and theoretical studies on the expansion of highly concentrated bacterial droplets into an ambient bacteria-free fluid.

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Chemically active Brownian particles with surface catalytic reactions may repel each other due to diffusiophoretic interactions in the reaction and product concentration fields. The system behavior can be described by a "chemical" coupling parameter Γ_{c} that compares the strength of diffusiophoretic repulsion to Brownian motion, and by a mapping to the classical electrostatic one component plasma (OCP) system. When confined to a constant-volume domain, body-centered cubic (bcc) crystals spontaneously form from random initial configurations when the repulsion is strong enough to overcome Brownian motion.

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A body submerged in active matter feels the swim pressure through a kinetic accumulation boundary layer on its surface. The boundary layer results from a balance between translational diffusion and advective swimming and occurs on the microscopic length scale . Here , D is the Brownian translational diffusivity, τ is the reorientation time and l = Uτ is the swimmer's run length, with U the swim speed [Yan and Brady, J.

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We use Brownian Dynamics (BD) simulations and continuum models to study the microstructures and mechanics in the colloidal film drying process. Colloidal suspensions are compressed between a planar moving interface and a stationary substrate. In the BD simulations, we develop a new Energy Minimization Potential-Free (EMPF) algorithm to enforce the hard-sphere potential in confined systems and to accurately measure the stress profile.

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We study the diffusion of a Brownian probe particle of size R in a dilute dispersion of active Brownian particles of size a, characteristic swim speed U_{0}, reorientation time τ_{R}, and mechanical energy k_{s}T_{s}=ζ_{a}U_{0}^{2}τ_{R}/6, where ζ_{a} is the Stokes drag coefficient of a swimmer. The probe has a thermal diffusivity D_{P}=k_{B}T/ζ_{P}, where k_{B}T is the thermal energy of the solvent and ζ_{P} is the Stokes drag coefficient for the probe. When the swimmers are inactive, collisions between the probe and the swimmers sterically hinder the probe's diffusive motion.

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