ABSTRACT
Geometrical constraints offer a promising strategy for assembling colloidal crystal structures that are not typically observed in bulk or under 2D conditions. Core-softened colloids, in particular, have emerged as versatile chemical building blocks with applications across various scientific and technological areas. In this study, we investigate the behavior of a core-softened model confined between two parallel walls. Employing molecular dynamics simulations, we analyze the system's response under extreme confinement, where only one or two layers of colloids are permitted. The system comprises particles modeled by a ramp-like potential confined within slit nanoslits created by two flat, purely repulsive walls with a lateral side L separated by a distance Lz. Through a systematic analysis of the phase behavior as Lz increases, or as the system undergoes decompression, for different values of L, we identified a mono-to-bilayer transition associated with changes in the colloidal structure. In the monolayer regime, we observed solid phases at lower densities than those observed in the 2D case. Importantly, we demonstrated that confinement at specific Lz values, allowing particle arrangement into two layers, can lead to the emergence of the square phase, which was not observed under monolayer or 2D conditions. By correlating thermodynamic, translational, and orientational ordering, as well as the dynamics of this confined colloidal system, our findings offer valuable insights into the utilization of geometrical constraints to induce and manipulate structural changes.
