Impact of non-reciprocal interactions on colloidal self-assembly with tunable anisotropy.

Non-reciprocal (NR) effective interactions violating Newton's third law occur in many biological systems, but can also be engineered in synthetic, colloidal systems. Recent research has shown that such NR interactions can have tremendous effects on the overall collective behavior and pattern formation, but can also influence aggregation processes on the particle scale. Here, we focus on the impact of non-reciprocity on the self-assembly of a colloidal system (originally passive) with anisotropic interactions whose character is tunable by external fields. In the absence of non-reciprocity, that is, under equilibrium conditions, the colloids form square-like and hexagonal aggregates with extremely long lifetimes yet no large-scale phase separation [Kogler et al., Soft Matter 11, 7356 (2015)], indicating kinetic trapping. Here, we study, based on Brownian dynamics simulations in 2D, an NR version of this model consisting of two species with reciprocal isotropic, but NR anisotropic interactions. We find that NR induces an effective propulsion of particle pairs and small aggregates ("active colloidal molecules") forming at the initial stages of self-assembly, an indication of the NR-induced non-equilibrium. The shape and stability of these initial clusters strongly depend on the degree of anisotropy. At longer times, we find, for weak NR interactions, large (even system-spanning) clusters where single particles can escape and enter at the boundaries, in stark contrast to the small rigid aggregates appearing at the same time in the passive case. In this sense, weak NR shortcuts the aggregation. Increasing the degree of NR (and thus, propulsion), we even observe large-scale phase separation if the interactions are weakly anisotropic. In contrast, systems with strong NR and anisotropy remain essentially disordered. Overall, the NR interactions are shown to destabilize the rigid aggregates interrupting self-assembly and phase separation in the passive case, thereby helping the system to overcome kinetic barriers.