Macromolecular crowding in chiral assembly of ellipsoidal nanoparticles

Anisotropic colloidal particles have the ability to self-assemble into cholesteric structures. We used molecular dynamics to simulate the self-assembly of ellipsoidal particles with the objective to establish a general framework to reveal the primary factors driving chiral interactions. To characterize these interactions, we introduce a characteristic parameter following the crowding factor (CF) theory. Our simulations and statistical analysis showed good agreement with the CF theory; at the early stages of the assembly process, the ellipsoidal particles go through a critical aggregation point followed by further clustering towards nematic order. Further, we demonstrate that in high CF conditions, small initial clusters may induce a chiral twist which subsequently forms a cholesteric structure with no directional preference in higher organization states.

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