Polymeric Moebius strips, characterized by their single-sided topology, exhibit remarkable optical and mechanical properties, making them promising candidates for advanced technological applications. However, the lack of well-established design principles and control mechanisms governing the formation of chiral morphologies has hindered their practical implementation. In this study, we present a tailored mesoscale molecular dynamics simulation strategy for chiral block copolymers to gain mechanistic insights into the formation and chirality transfer of polymeric Moebius strips. The results reveal that the solvent-philic achiral blocks form a segregated corona layer, creating a local microenvironment dynamically shaped by interfacial interactions, within which the chiral blocks self-assemble. This microenvironment promotes the emergence of cholesteric liquid crystalline order within the chiral block domains, which in turn leads to a two-step chirality transfer process. Specifically, chirality transfer occurs across three distinct hierarchical levels during Moebius strip formation: from the configurational point chirality of the monomers, to the conformational helical chirality of the chiral blocks, and ultimately to the assembly chirality of the Moebius strips. These uncovered mechanisms provide a comprehensive understanding of the formation and chirality transfer in polymeric Moebius strips, thereby establishing a critical foundation for the rational design of advanced chiral polymeric materials.
Li et al. (Wed,) studied this question.