Year: 2026
Type: preprint
Abstract: Creating synthetic systems that autonomously form complex patterns remains a frontier challenge in chemistry and materials science. Here, we present a redox-responsive supramolecular system in which coupled changes in chemical state, assembly, and transport generate spatiotemporal patterns through density-driven chemoconvection. Charge-transfer complexes of pyranine and viologen derivatives undergo reversible redox-controlled assembly–disassembly cycles, producing composition-dependent buoyancy that drive convective flows and feeds back into the evolving assembly distribution. Molecular amphiphilicity and supramolecular assembly morphology tune the resulting pattern type, dot-, stripe-, and flower-like structures without external fields. Finite-element simulations reproduce the observed chemoconvective dynamics, while linear stability analysis predicts the onset conditions and its characteristic wavelength. A weakly nonlinear analysis further identifies reduced translational diffusivity of elongated assemblies as a mechanism that weakens hexagonal mode selection and favors anisotropic near-onset states. These results provide a molecular-to-macroscopic framework for coupling supramolecular organization with chemically driven hydrodynamic pattern formation.
Source: ChemRxiv
Language: English
Subfield: Biomaterials
Field: Materials Science
Domain: Physical Sciences
Open Access status: green
OpenAlex ID: W7212072817