Phase coexistence in a monolayer of active particles induced by Marangoni flows

Abstract

Thermally or chemically active colloids generate thermodynamic gradients in the solution in which they are immersed and thereby induce hydrodynamic flows that affect their dynamical evolution. Here we study a mean-field model for the many-body dynamics of a monolayer of spherically symmetric active particles located at a fluid–fluid interface. Due to the spherical symmetry, the particles do not self-propel. Instead, the dynamics is driven by the long-ranged Marangoni flows, due to the response of the interface to the activity of the particles, which compete with the direct interaction between particles. We demonstrate analytically that, in spite of the intrinsic out-of-equilibrium character of the system, the monolayer evolves to a “pseudoequilibrium” state, in which the Marangoni flows force the coexistence of the thermodynamic phases associated to the direct interaction. In particular, we study the most interesting case of a r⁻³ soft repulsion that models electrostatic or magnetic interparticle forces. For a sufficiently large average density, two-dimensional phase transitions (freezing from liquid to hexatic, and melting from solid to hexatic) should be observable in a radially stratified, “onion-like” structure within the monolayer. Furthermore, the analysis allows us to conclude that, while the activity may be too weak to allow direct detection of such induced Marangoni flows, it is relevant as a collective effect in the emergence of the experimentally observable spatial structure of phase coexistences noted above. Finally, the relevance of these results for potential experimental realizations is critically discussed.