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Ahmad K. Omar

Publications and source records attributed to Ahmad K. Omar.

At least 19 recordsLinked to original sources

Active Particles Destabilize Passive Membranes

We present a theory for the interaction between active particles and a passive flexible membrane. By explicitly solving for the pressure exerted by the active particles, we show that they reduce the membrane tension and bending modulus and introduce novel non-local contributions to the membrane mechanics. This theory predicts activity-induced instabilities and their morphology are in agreement with recent experimental and simulation data.

cond-mat.soft↗

Emergent nonreciprocity in open thermodynamically-consistent chemical reaction networks

Nonreciprocity, a hallmark of nonequilibrium systems, can generate dynamics not possible near thermodynamic equilibrium, including oscillatory and rotating patterns. The onset of temporal oscillations is often evident in linearized dynamics, where nonreciprocity appears as complex eigenvalues of an asymmetric Jacobian. Here, we show that the topology of open, thermodynamically-consistent chemical reaction networks can result in oscillatory instabilities near nonequilibrium steady states. These instabilities arise from chemostat-induced breaking of Onsager reciprocity, while the local equilibrium hypothesis preserves the variational structure of the dissipative part of the dynamics. Numerical results confirm that such nonreciprocity in reaction-diffusion systems produces oscillatory dynamics that nevertheless minimize a free energy.

cond-mat.stat-mech↗

Hexatic Order Coupled with Thermal Noise Produces Bubbles in Two-Dimensional Active Matter

The phase separation of purely-repulsive particles induced by self-propulsion is among the most well-studied non-equilibrium phase transitions. However, some notable features of this transition remain open questions, including the origin of bubbles within the dense phase in two dimensions. Various explanations have been proposed, ranging from a reversal of the Ostwald ripening process to topological defects at the borders of hexatic domains. We present particle-based simulations that disentangle the effect of hexatic domains on the bubble size and number distribution through the introduction of polydispersity. While hexatic order is found to be necessary for bubble formation, we also identify thermal translational noise is required for bubble generation. Intriguingly, the magnitude of the thermal noise needed for bubble formation can be remarkably small in comparison with the particle activity but cannot be identically zero. The cooperative motion evidenced within the dense phase of the thermal hexatic domains may may be necessary for bubble production.

cond-mat.soft↗

Tunable Nanostructures from Inverse Surfactants

Hierarchical materials in the natural world are often made through the self-assembly of amphiphilic molecules. Achieving similar structural complexity in synthetic materials requires understanding how various molecular parameters affect assembly behavior. In recent years, inverse surfactants -- molecules with hydrophobic head groups and hydrophilic macromolecular tails -- have been shown to self-assemble into supramolecular assemblies in aqueous solutions that show promise for a number of applications, including drug delivery. Here, we build an understanding of the morphological phase diagram of inverse surfactants using insights from scattering experiments, computer simulations, and statistical mechanics. The scattering and simulation results reveal that changing the head-group size is an important molecular knob in controlling morphological transitions. The molecular size ratio of the hydrophobic group to the hydrophilic emerges as a crucial dimensionless quantity in our theory and plays a determining role in setting the micelle structure and the transition from mesoscale to macroscale aggregates. Our minimal theory is able to qualitatively explain the key features of the morphological phase diagram, including the prevalence of fiber-like structures in comparison to spherical and planar micelles. Together, these findings provide a more complete picture for the molecular dependencies of assemblies of inverse surfactants, which we hope may aid in the de novo design of supramolecular structures.

cond-mat.soft↗

Critical Motility-Induced Phase Separation in Three Dimensions is Consistent with Ising Universality

Identifying the universality class of critical active phase transitions has been the subject of recent interest and controversy. Resolving these controversies will require robust numerical investigations to determine whether active critical exponents point to novel universality classes or are consistent with established ones. Here, we conduct large-scale computer simulations and a finite-size scaling analysis of the motility-induced phase separation (MIPS) of active Brownian hard spheres in three dimensions (3D), finding that the static and dynamic critical exponents all closely match those of the 3D Ising universality class with a conserved scalar order parameter. This finding is corroborated by a fluctuating hydrodynamic description of the critical dynamics of the order parameter field which flows to the Wilson-Fisher fixed point in three dimensions. Our work suggests that 3D MIPS and likely the entire phase diagram of active Brownian hard spheres is similar to that of molecular passive fluids despite the absence of Boltzmann statistics.

cond-mat.stat-mech↗

Dynamic Permeability in Metastable Droplet Interfacial Bilayers

Membrane pores are implicated in several critical functions, including cell fusion and the transport of signaling molecules for intercellular communication. However, these structural features are often difficult to probe directly. Droplet interfacial bilayers offer a synthetic platform to study such membrane properties. We develop a theory that links size-selective transport across a metastable membrane with its transient structural properties. The central quantity of our theory is a dynamic permeability that depends on the mechanism of pore growth, which controls the transient distribution of pore sizes in the membrane. We present a mechanical perspective to derive pore growth dynamics and the resulting size distribution for growth \textit{via} Ostwald ripening and discuss how these dynamics compare to other growth mechanisms such as coalescence and growth through surfactant desorption. We find scaling relations between the transported particle size, the pore growth rate, and the time for a given fraction of particles to cross the membrane, from which one may deduce the dominant mechanism of pore growth, as well as material properties and structural features of the membrane. Finally, we suggest experiments using droplet interfacial bilayers to validate our theoretical predictions.

cond-mat.soft↗

Self-assembly of anisotropic particles on curved surfaces

The surface curvature of membranes, interfaces, and substrates plays a crucial role in shaping the self-assembly of particles adsorbed on these surfaces. However, little is known about the interplay between particle anisotropy and surface curvature and how they couple to alter the free energy landscape of particle assemblies. Using molecular dynamics simulations, we investigate the effect of prescribed curvatures on a quasi-2D assembly of anisotropic patchy particles. By varying curvature and surface coverage, we uncover a rich geometric phase diagram, with curvature inducing ordered structures entirely absent on planar surfaces. Large spatial domains of ordered structures can contain hidden microdomains of orientational textures imprinted by the surface on the assembly. The dynamical landscape is also reshaped by surface curvature, with a glass-like state emerging at modest densities and high curvature. Changes to the symmetry of the surface curvature are found to result in distinct structures, including phases with mesoscale ordering. Our findings show that the coupling between surface curvature and particle geometry opens an unexplored space of morphologies and structures that can be exploited for material design.

cond-mat.soft↗

The Mechanics of Nucleation and Growth and the Surface Tensions of Active Matter

Homogeneous nucleation, a textbook transition path for phase transitions, is typically understood on thermodynamic grounds through the prism of classical nucleation theory. However, recent studies have suggested the applicability of classical nucleation theory to systems far from equilibrium. In this Article, we formulate a purely mechanical perspective of homogeneous nucleation and growth, elucidating the criteria for the properties of a critical nucleus without appealing to equilibrium notions. Applying this theory to active fluids undergoing motility-induced phase separation, we find that nucleation proceeds in a qualitatively similar fashion to equilibrium systems, with concepts such as the Gibbs-Thomson effect and nucleation barriers remaining valid. We further demonstrate that the recovery of such concepts allows us to extend classical theories of nucleation rates and coarsening dynamics to active systems upon using the mechanically-derived definitions of the nucleation barrier and surface tensions. Three distinct surface tensions -- the mechanical, capillary, and Ostwald tensions -- play a central role in our theory. While these three surface tensions are identical in equilibrium, our work highlights the distinctive role of each tension in the stability of active interfaces and the nucleation and growth of motility-induced phases.

cond-mat.soft↗

Multicomponent Linear Transport in the Absence of Local Equilibrium

The linear laws of transport phenomena are central in our description of irreversible processes in systems across the physical sciences. Linear irreversible thermodynamics allows for the identification of the underlying forces driving transport and the structure of the relevant transport coefficients for systems that are locally in equilibrium. Increasingly, linear relations are found to describe transport in systems in which a local equilibrium hypothesis is unlikely to hold. Here, we derive a mechanical theory of multicomponent transport without appealing to equilibrium notions. Our theory for the Onsager transport tensor highlights the general breakdown of the familiar Onsager reciprocal relations and Einstein relations when a local equilibrium is absent. The procedure outlined is applied to a variety of systems, including passive systems, mixtures with nonreciprocal interactions, electrolytes under an electric field, and active systems, and can be straightforwardly used to understand other transport processes. The framework further provides a basis to extend numerical approaches for computing the transport coefficients of nonequilibrium systems, as is demonstrated for a system with nonreciprocal interactions.

cond-mat.stat-mech↗

Theory for the Anomalous Phase Behavior of Inertial Active Brownian Particles

In contrast to equilibrium systems, inertia can profoundly impact the phase behavior of active systems. This has been made particularly evident in recent years, with motility-induced phase separation (MIPS) exhibiting several intriguing dependencies on translational inertia. Here we report extensive simulations characterizing the phase behavior of inertial active matter and develop a mechanical theory for the complete phase diagram without appealing to equilibrium notions. Our theory qualitatively captures all aspects of liquid-gas coexistence, including the critical value of inertia above which MIPS ceases. Notably, our findings highlight that particle softness, and not inertia, is responsible for the MIPS reentrance effect at the center of a proposed active refrigeration cycle.

cond-mat.soft↗

Theory of Nonequilibrium Crystallization and the Phase Diagram of Active Brownian Spheres

The crystallization of hard spheres at equilibrium is perhaps the most familiar example of an entropically-driven phase transition. In recent years, it has become clear that activity can dramatically alter this order-disorder transition in unexpected ways. The theoretical description of active crystallization has remained elusive as the traditional thermodynamic arguments that shape our understanding of passive freezing are inapplicable to active systems. Here, we develop a statistical mechanical description of the one-body density field and a nonconserved order parameter field that represents local crystalline order. We develop equations of state, guided by computer simulations, describing the crystallinity field which result in shifting the order-disorder transition to higher packing fractions with increasing activity. We then leverage our recent dynamical theory of coexistence to construct the full phase diagram of active Brownian spheres, quantitatively recapitulating both the solid-fluid and liquid-gas coexistence curves and the solid-liquid-gas triple point.

cond-mat.stat-mech↗

Theory of Nonequilibrium Coexistence with Coupled Conserved and Nonconserved Order Parameters

Phase separation routinely occurs in both living and synthetic systems. These phases are often complex and distinguished by features including crystallinity, nematic order, and a host of other nonconserved order parameters. For systems at equilibrium, the phase boundaries that characterize these transitions can be straightforwardly determined through the framework of thermodynamics. The prevalence of phase separation in active and driven systems motivates the need for a genuinely nonequilibrium theory for the coexistence of complex phases. Here, we develop a dynamical theory of coexistence when both conserved and nonconserved order parameters are present, casting coexistence criteria into the familiar form of equality of state functions. Our theory generalizes thermodynamic notions such as the chemical potential and Gibbs-Duhem relation to systems out of equilibrium. While these notions may not exist for all nonequilibrium systems, we numerically verify their existence for a variety of systems by introducing the phenomenological Active Model C+. We hope our work aids in the development of a comprehensive theory of high-dimensional nonequilibrium phase diagrams.

cond-mat.stat-mech↗

Theory of Nonequilibrium Multicomponent Coexistence

Multicomponent phase separation is a routine occurrence in both living and synthetic systems. Thermodynamics provides a straightforward path to determine the phase boundaries that characterize these transitions for systems at equilibrium. The prevalence of phase separation in complex systems outside the confines of equilibrium motivates the need for a genuinely nonequilibrium theory of multicomponent phase coexistence. Here, we develop a mechanical theory for coexistence that casts coexistence criteria into the familiar form of equality of state functions. Our theory generalizes traditional equilibrium notions such as the species chemical potential and thermodynamic pressure to systems out of equilibrium. Crucially, while these notions may not be identifiable for all nonequilibrium systems, we numerically verify their existence for a variety of systems by introducing the phenomenological Multicomponent Active Model B+. Our work establishes an initial framework for understanding multicomponent coexistence that we hope can serve as the basis for a comprehensive theory for high-dimensional nonequilibrium phase transitions.

cond-mat.stat-mech↗

Phase Separation, Capillarity, and Odd Surface Flows in Chiral Active Matter

Active phase separations evade canonical thermodynamic descriptions and have thus challenged our understanding of coexistence and interfacial phenomena. Considerable progress has been made towards a non-equilibrium theoretical description of these traditionally thermodynamic concepts. Spatial parity symmetry is conspicuously assumed in much of this progress, despite the ubiquity of chirality in experimentally realized systems. In this Letter, we derive a theory for the phase coexistence and interfacial fluctuations of a system which microscopically violates spatial parity. We find suppression of the phase separation as chirality is increased as well as the development of steady-state currents tangential to the interface dividing the phases. These odd flows are irrelevant to stationary interfacial properties, with stability, capillary fluctuations, and surface area minimization determined entirely by the capillary surface tension. Using large-scale Brownian dynamics simulations, we find excellent agreement with our theoretical scaling predictions.

cond-mat.soft↗

Theory of Capillary Tension and Interfacial Dynamics of Motility-Induced Phases

The statistical mechanics of equilibrium interfaces has been well-established for over a half century. In the last decade, a wealth of observations have made increasingly clear that a new perspective is required to describe interfaces arbitrarily far from equilibrium. In this work, beginning from microscopic particle dynamics that break time-reversal symmetry, we systematically derive the interfacial dynamics of coexisting motility-induced phases. Doing so allows us to identify the athermal energy scale that excites interfacial fluctuations and the nonequilibrium surface tension that resists these excitations. Our theory identifies that, in contrast to equilibrium fluids, this active surface tension contains contributions arising from nonconservative forces which act to suppress interfacial fluctuations and, crucially, is distinct from the mechanical surface tension of Kirkwood and Buff. We find that the interfacial stiffness scales linearly with the intrinsic persistence length of the constituent active particle trajectories, in agreement with simulation data. We demonstrate that at wavelengths much larger than the persistence length, the interface obeys surface area minimizing Boltzmann statistics with our derived nonequilibrium interfacial stiffness playing an identical role to that of equilibrium systems.

cond-mat.soft↗

The Flux Hypothesis for Odd Transport Phenomena

Onsager's regression hypothesis makes a fundamental connection between macroscopic transport phenomena and the average relaxation of spontaneous microscopic fluctuations. This relaxation, however, is agnostic to odd transport phenomena, in which fluxes run orthogonal to the gradients driving them. To account for odd transport, we generalize the regression hypothesis, postulating that macroscopic linear constitutive laws are, on average, obeyed by microscopic fluctuations, whether they contribute to relaxation or not. From this "flux hypothesis," Green-Kubo and reciprocal relations follow, elucidating the separate roles of broken time-reversal and parity symmetries underlying various odd transport coefficients. As an application, we derive and verify the Green-Kubo relation for odd collective diffusion in chiral active matter, first in an analytically-tractable model and subsequently through molecular dynamics simulations of concentrated active spinners.

cond-mat.stat-mech↗

Phase Coexistence Implications of Violating Newton's Third Law

Newton's third law, actio = reactio, is a foundational statement of classical mechanics. However, in natural and living systems, this law appears to be routinely violated for constituents interacting in a nonequilibrium environment. Here, we use computer simulations to explore the macroscopic phase behavior implications of breaking microscopic interaction reciprocity for a simple model system. We consider a binary mixture of attractive particles and introduce a parameter which is a continuous measure of the degree to which interaction reciprocity is broken. In the reciprocal limit, the species are indistinguishable and the system phase separates into domains with distinct densities and identical compositions. Increasing nonreciprocity is found to drive the system to explore a rich assortment of phases, including phases with strong composition asymmetries and three-phase coexistence. Many of the states induced by these forces, including traveling crystals and liquids, have no equilibrium analogue. By mapping the complete phase diagram for this model system and characterizing these unique phases, our findings offer a concrete path forward towards understanding how nonreciprocity shapes the structures found in living systems and how this might be leveraged in the design of synthetic materials.

cond-mat.soft↗

Mechanical Theory of Nonequilibrium Coexistence and Motility-Induced Phase Separation

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. The core idea is that the mechanical forces within the interface separating two coexisting phases uniquely determine coexistence criteria, regardless of whether a system is in equilibrium or not. We demonstrate the power and utility of this theory by applying it to active Brownian particles, predicting a quantitative phase diagram for motility-induced phase separation in both two and three dimensions. This formulation additionally allows for the prediction of novel interfacial phenomena, such as an increasing interface width while moving deeper into the two-phase region, a uniquely nonequilibrium effect confirmed by computer simulations. The self-consistent determination of bulk phase behavior and interfacial phenomena offered by this mechanical perspective provide a concrete path forward towards a general theory for nonequilibrium phase transitions.

cond-mat.stat-mech↗