Two-Step Chirality Transfer to Twisted Assemblies: Synergistic Interplay of Chiral and Aggregation Interactions.

Chirality plays a pivotal role in both the origin of life and the self-assembly of materials. However, the governing principles behind chirality transfer in hierarchical self-assembly across multiple length scales remain elusive. Here, we propose a concise and versatile simulation strategy using the patchy particle chain model to investigate the self-assembly of rods interacting through chiral and aggregation interactions. We reveal that chiral interaction possessing an entropic nature, amplifies the fluctuations and twists in the alignment of rods, while aggregation interaction serves as a foundational platform for aggregation and assembly. When both interactions exhibit moderate absolute and relative values, their synergistic interplay facilitates the chirality transfer from rods to assemblies, resulting in the formation of chiral mesoscale ordered structures. Furthermore, we observe a two-step chirality transfer process by monitoring the formation kinetics of the twisted assemblies. This work not only provides a comprehensive insight into chirality transfer mechanisms, but also introduces a versatile mesoscale simulation framework for exploring the role of chirality in hierarchical self-assembly.