Self-limiting assembly of curvature-frustrated, shell colloids

Geometric frustration in self-assembling systems can propagate local inter-subunit shape misfits to large scale strain gradients yielding finitely sized, self-limiting structures in equilibrium. Recently, models of soft, cylindrical, colloidal shells established a transition from self-limiting to unlimited self-stacking beyond a critical attraction range at zero temperature. However, short-ranged attractions may promote long assembly timescales challenging the feasibility of achieving self-limitation from an initially dispersed state out of equilibrium at finite temperature. Here, we propose a coarse-grained numerical model of frustrated colloidal shells and explore the thermodynamic conditions necessary for successful assembly. We find the regimes of temperature, concentration and attraction range for optimal assembly kinetics with finite temperature molecular dynamics simulations and further investigate the roles of subunit shape and entropy in avoiding kinetic traps which inhibit assembly. In conjunction with ongoing experiments of curved, DNA origami shells, we test theoretical predictions of resulting assembly size distributions and provide critical guidance for further experimental realizations of self-limiting frustrated particle systems.