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Ahmad K. Omar

Publications and source records attributed to Ahmad K. Omar.

26 records · Page 2Linked to original sources

Remembering the work of Phillip L. Geissler: A coda to his scientific trajectory

Phillip L. Geissler made important contributions to the statistical mechanics of biological polymers, heterogeneous materials, and chemical dynamics in aqueous environments. He devised analytical and computational methods that revealed the underlying organization of complex systems at the frontiers of biology, chemistry, and materials science. In this retrospective, we celebrate his work at these frontiers.

cond-mat.stat-mech↗

Ballistic Ejection of Microdroplets from Overpacked Interfacial Assemblies

Spontaneous emulsification, resulting from the assembly and accumulation of surfactants at liquid-liquid interfaces, is an interfacial instability where microdroplets are generated and diffusively spread from the interface until complete emulsification. Here, we show that an external magnetic field can modulate the assembly of paramagnetic nanoparticle surfactants (NPSs) at liquid-liquid interfaces and trigger an oversaturation in the areal density of the NPSs at the interface, as evidenced by a marked reduction in the interfacial tension, γ, and corroborated with a magnetostatic continuum theory. Despite the significant reduction in γ, the presence of the magnetic field does not cause stable interfaces to become unstable. Upon rapid removal of the field, however, an explosive ejection of a plume of microdroplets from the surface occurs, a dynamical interfacial instability which is termed explosive emulsification. This explosive event rapidly reduces the areal density of the NPSs to its pre-field level, stabilizing the interface. The ability to externally suppress or trigger the explosive emulsification and controlled generation of tens of thousands of microdroplets, uncovers an efficient energy storage and release process, that has potential applications for controlled and directed delivery of chemicals and remotely controlled soft microrobots, taking advantage of the ferromagnetic nature of the microdroplets.

cond-mat.soft↗

Tuning Nonequilibrium Phase Transitions with Inertia

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. This effect appears to be general for a wide class of active systems, including those driven by deterministic time-dependent external fields, whose nonequilibrium patterns ultimately disappear with increasing inertia. The path to this effective equilibrium limit can be complex, with finite inertia sometimes acting to accentuate nonequilibrium transitions. The restoration of near equilibrium statistics can be understood through the conversion of active momentum sources to passive-like stresses. Unlike truly equilibrium systems, the effective temperature is now density dependent, the only remnant of the nonequilibrium dynamics. This density-dependent temperature can in principle introduce departures from equilibrium expectations, particularly in response to strong gradients. Our results provide additional insight into the effective temperature ansatz while revealing a mechanism to tune nonequilibrium phase transitions.

cond-mat.soft↗

Topological Forces in a Model System for Reptation Dynamics

We construct a micromechanical version of an early model for topologically constrained polymers -- a 2D chain amongst point-like uncrossable obstacles -- which allows us to explicitly elucidate the role of topological forces beyond confining the chain to a curvilinear tube-like path. Our simulations reveal that linear relaxation of the contour length \textit{along the tube} is slowed down by the presence of topological forces that can be considered as additional effective topological ``friction'' in quiescence. However, this perspective fails in predicting the strong forces that resist the imposed curvilinear motion of the chain during nonlinear startup microrheology. These entropic forces are nonlocal in nature and result from an unexpected coupling between orientational and longitudinal dynamics.

cond-mat.soft↗

Phase Diagram of Active Brownian Spheres: Crystallization and the Metastability of Motility-Induced Phase Separation

Motility-induced phase separation (MIPS), the phenomenon in which purely repulsive active particles undergo a liquid-gas phase separation, is among the simplest and most widely studied examples of a nonequilibrium phase transition. Here, we show that states of MIPS coexistence are in fact only metastable for three-dimensional active Brownian particles over a very broad range of conditions, decaying at long times through an ordering transition we call active crystallization. At an activity just above the MIPS critical point, the liquid-gas binodal is superseded by the crystal-fluid coexistence curve, with solid, liquid, and gas all coexisting at the triple point where the two curves intersect. Nucleating an active crystal from a disordered fluid, however, requires a rare fluctuation that exhibits the nearly close-packed density of the solid phase. The corresponding barrier to crystallization is surmountable on a feasible timescale only at high activity, and only at fluid densities near maximal packing. The glassiness expected for such dense liquids at equilibrium is strongly mitigated by active forces, so that the lifetime of liquid-gas coexistence declines steadily with increasing activity, manifesting in simulations as a facile spontaneous crystallization at extremely high activity.

cond-mat.soft↗

Dynamic Overlap Concentration Scale of Active Colloids

By introducing the notion of a dynamic overlap concentration scale, we identify universal and previously unreported features of the mechanical properties of active colloids. These features are codified by recognizing that the characteristic length scale of an active particle's trajectory, the run-length, introduces a new concentration scale $ϕ^*$. Large-scale simulations of repulsive active Brownian particles (ABPs) confirm that this new run-length dependent concentration, which is the trajectory-space analogue of the overlap concentration in polymer solutions, delineates distinct concentration regimes in which interparticle collisions alter particle trajectories. Using $ϕ^*$ and concentration scales associated with colloidal jamming, the mechanical equation-of-state for ABPs can be collapsed onto a set of principal curves that contain a number of previously overlooked features. The inclusion of these features qualitatively alters previous predictions of the behavior for active colloids as we demonstrate by computing the spinodal for a suspension of purely-repulsive ABPs. Our findings suggest that dynamic overlap concentration scales should be of great utility in unraveling the behavior of active and driven systems.

cond-mat.soft↗

Microscopic Origins of the Swim Pressure and the Anomalous Surface Tension of Active Matter

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 \textit{extremely negative} surface tension between phase separated active particles. Here, we demonstrate that this contradiction stems from the fact that the swim pressure \textit{is not a true pressure}. At a boundary or interface, the reduction in particle swimming generates a net active force density -- an entirely \textit{self-generated body force}. The pressure at the boundary, which was previously identified as the swim pressure, is in fact an elevated (relative to the bulk) value of the \textit{traditional particle pressure} that is generated by this interfacial force density. Recognizing this unique mechanism for stress generation allows us to define a much more physically plausible surface tension. We clarify the utility of the swim pressure as an "equivalent pressure" (analogous to those defined from electrostatic and gravitational body forces) and the conditions in which this concept can be appropriately applied.

cond-mat.soft↗

Swimming to Stability: Structural and Dynamical Control via Active Doping

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. Moreover, by carefully tuning the active particle properties (the propulsive swim force and persistence length) in comparison to those of the gel, the active particles may induce depletion-like forces between the constituent particles of the gel despite there being no geometric size asymmetry between the particles. These resulting forces can rapidly push the system toward disparate regions of phase space. Intriguingly, the state of the material can be altered by tuning macroscopic transport properties such as the solvent viscosity. Our findings highlight the potential wide-ranging structural and kinetic control facilitated by varying the dynamical properties of a remarkably small fraction of driven particles embedded in a host material.

cond-mat.soft↗