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Despite a mounting evidence that the same gradients which active colloids use for swimming, induce important cross-interactions (phoretic interaction), they are still ignored in most many-body descriptions, perhaps to avoid complexity and a zoo of unknown parameters. Here we derive a simple model, which reduces phoretic far-field interactions to a pair-interaction whose strength is mainly controlled by one genuine parameter (swimming speed). The model suggests that phoretic interactions are generically important for autophoretic colloids (unless effective screening of the phoretic fields is strong) and should dominate over hydrodynamic interactions for the typical case of half-coating and moderately nonuniform surface mobilities. Unlike standard minimal models, but in accordance with canonical experiments, our model generically predicts dynamic clustering in active colloids at low density. This suggests that dynamic clustering can emerge from the interplay of screened phoretic attractions and active diffusion.
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We study effective two- and three-body interactions between non-active colloidal inclusions in an active bath of chiral or non-chiral particles, using Brownian Dynamics simulations within a standard, two-dimensional model of disk-shaped inclusions and active particles. In a non-chiral active bath, we first corroborate previous findings on effective two-body repulsion mediated between the inclusions by elucidating the detailed non-monotonic features of the two-body force profiles, including a primary maximum, and a secondary hump at larger separations that was not previously reported. We then show that these features arise directly from the formation, and sequential overlaps, of circular layers (or rings) of active particles around the inclusions, as the latter are brought to small surface separations. These rings extend to radial distances of a few active-particle radii from the surface of inclusions, giving the hard-core inclusions relatively thick, soft, repulsive shoulders, whose multiple overlaps then enable significant (non-pairwise) three-body forces in both non-chiral and chiral active baths. The resulting three-body forces can even exceed the two-body forces in magnitude and display distinct repulsive and attractive regimes at intermediate to large self-propulsion strengths. In a chiral active bath, we show that, while active particles still tend to accumulate at the immediate vicinity of the inclusions, they exhibit strong depletion from the intervening region between the inclusions, and partial depletion from relatively thick, circular, zones further away from the inclusions. In this case, the effective, predominantly repulsive, interactions between the inclusions turn to active, chirality-induced, depletion-type attractions, acting over an extended range of separations.
The glass transition remains unclarified in condensed matter physics. Investigating the mechanical properties of glass is challenging because any global deformation that may result in shear rejuvenation requires an astronomical relaxation time. Moreover, it is well known that a glass is heterogeneous and a global perturbation cannot explore local mechanical/transport properties. However, an investigation based on a local probe, i.e. microrheology, may overcome these problems. Here, we establish active microrheology of a bulk metallic glass: a probe particle driven into host medium glass. This is a technique amenable for experimental investigations. We show that upon cooling the microscopic friction exhibits a second-order phase transition; this sheds light on the origin of friction in heterogeneous materials. Further, we provide distinct evidence to demonstrate that a strong relationship exists between the microscopic dynamics of the probe particle and the macroscopic properties of the host medium glass. These findings establish active microrheology as a promising technique for investigating the local properties of bulk metallic glass.
Colloids that interact via a short-range attraction serve as the primary building blocks for a broad range of self-assembled materials. However, one of the well-known drawbacks to this strategy is that these building blocks rapidly and readily condense into a metastable colloidal gel. Using computer simulations, we illustrate how the addition of a small fraction of purely repulsive self-propelled colloids, a technique referred to as active doping, can prevent the formation of this metastable gel state and drive the system toward its thermodynamically favored crystalline target structure. The simplicity and robust nature of this strategy offers a systematic and generic pathway to improving the self-assembly of a large number of complex colloidal structures. We discuss in detail the process by which this feat is accomplished and provide quantitative metrics for exploiting it to modulate self-assembly. We provide evidence for the generic nature of this approach by demonstrating that it remains robust under a number of different anisotropic short-ranged pair interactions in both two and three dimensions. In addition, we report on a novel microphase in mixtures of passive and active colloids. For a broad range of self-propelling velocities, it is possible to stabilize a suspension of fairly monodisperse finite-size crystallites. Surprisingly, this microphase is also insensitive to the underlying pair interaction between building blocks. The active stabilization of these moderately-sized monodisperse clusters is quite remarkable and should be of great utility in the design of hierarchical self-assembly strategies. This work further bolsters the notion that active forces can play a pivotal role in directing colloidal self-assembly.
In recent years significant attention has been attracted to proposals which utilize DNA for nanotechnological applications. Potential applications of these ideas range from the programmable self-assembly of colloidal crystals, to biosensors and nanoparticle based drug delivery platforms. In Chapter I we introduce the system, which generically consists of colloidal particles functionalized with specially designed DNA markers. The sequence of bases on the DNA markers determines the particle type. Due to the hybridization between complementary single-stranded DNA, specific, type-dependent interactions can be introduced between particles by choosing the appropriate DNA marker sequences. In Chapter II we develop a statistical mechanical description of the aggregation and melting behavior of particles with DNA-mediated interactions. In Chapter III a model is proposed to describe the dynamical departure and diffusion of particles which form reversible key-lock connections. In Chapter IV we propose a method to self-assemble nanoparticle clusters using DNA scaffolds. A natural extension is discussed in Chapter V, the programmable self-assembly of nanoparticle clusters where the desired cluster geometry is encoded using DNA-mediated interactions. In Chapter VI we consider a nanoparticle based drug delivery platform for targeted, cell specific chemotherapy. In Chapter VII we present prospects for future research: the connection between DNA-mediated colloidal crystallization and jamming, and the inverse problem in self-assembly.
We introduce a representative minimal model for phoretically interacting active colloids. Combining kinetic theory, linear stability analyses, and a general relation between self-propulsion and phoretic interactions in auto-diffusiophoretic and auto-thermophoretic Janus colloids collapses the parameter space to two dimensions: area fraction and Peclet number. This collapse arises when the lifetime of the self-generated phoretic fields is not too short, and leads to a universal phase diagram showing that phoretic interactions {it generically} induce pattern formation in typical Janus colloids, even at very low density. The resulting patterns include waves and dynamic aggregates closely resembling the living clusters found in experiments on dilute suspension of Janus colloids.
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