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PreprintCC BYChemRxiv

Chemically Fueled Spatiotemporal Patterns from Charge-transfer Supramolecular Assembly

  • Surbhi Sharma1
  • Aritra K. Mukhopadhyay2
  • Mohit Kumar1
  • Jessica Erlenbusch1
  • Ankit Sakhuja1
  • Benno Liebchen2
  • Shikha Dhiman1
  1. 1Johannes Gutenberg University Mainz
  2. 2Institute for Condensed Matter Physics, Technische Universität Darmstadt, Hochschulstraße 8, Darmstadt, Germany, 64289
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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.

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Cite

BibTeXRIS
BibTeX
@misc{sharma2026chemically,
  title = {{Chemically Fueled Spatiotemporal Patterns from Charge-transfer Supramolecular Assembly}},
  author = {Surbhi Sharma and Aritra K. Mukhopadhyay and Mohit Kumar and Jessica Erlenbusch and Ankit Sakhuja and Benno Liebchen and Shikha Dhiman},
  howpublished = {ChemRxiv},
  year = {2026},
  month = sep,
  doi = {10.26434/chemrxiv-2024-r3l1b/v2},
  url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv-2024-r3l1b/v2},
  note = {CC BY},
}
RIS
TY  - UNPB
TI  - Chemically Fueled Spatiotemporal Patterns from Charge-transfer Supramolecular Assembly
AU  - Surbhi Sharma
AU  - Aritra K. Mukhopadhyay
AU  - Mohit Kumar
AU  - Jessica Erlenbusch
AU  - Ankit Sakhuja
AU  - Benno Liebchen
AU  - Shikha Dhiman
PY  - 2026
DA  - 2026/09/08
PB  - ChemRxiv
DO  - 10.26434/chemrxiv-2024-r3l1b/v2
UR  - https://chemrxiv.org/doi/full/10.26434/chemrxiv-2024-r3l1b/v2
AB  - 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.
ER  -