A bottom-up design strategy for controllable self-assembly based on the isotropic double-well potential

Abstract

Controllable self-assembly of particles or atoms is still challenging in the synthesis of materials with desirable properties that are highly relevant to the microscopic structures determined by the interparticle interactions. To gain insight into how the interactions affect the self-assembly, we designed various kinds of isotropic double-well potentials and simulated the motion of the particles. By controlling the depth and location of the potential wells and the height of the barriers, we studied their effects on the aggregation structures and the related microscopic kinetic processes. We identified five aggregation patterns at different temperatures and eight kinds of crystals, including Frank–Kasper phases, and observed the expansion or contraction of crystals. We found that the system usually stays in a sparse configuration at very low or very high temperatures. The particles typically assemble into a loosely packed cluster at medium temperatures and then deplete into a tightly packed state with a specific pattern. These phenomena can be explained from the perspective of energy. In contrast, very few structures could be obtained for the system guided by a single-well potential under the same simulation conditions. Thus, the interparticle interactions driven by the double-well potential greatly enrich the possible packing morphology of the system. The information obtained from this work helps us to understand how to achieve a specific self-assembled architecture through a reasonable selection of materials.