Nucleotides trigger the spontaneous emergence of hierarchical nanolamellar architectures in coacervate-like polyelectrolyte multilayers
4 affiliations
- 1Institut Charles Sadron (UPR22, 23 rue du Loess, Strasbourg Cedex, France, BP 84047
- 2CNRS, 25 rue Becquerel, Strasbourg Cedex, France, 67087
- 3CRBS, 1 rue Eugène Boeckel, Strasbourg, France, 67000
- 4Faculté de Chirurgie Dentaire, Université de Strasbourg, 8 rue Sainte Elisabeth, Strasbourg, France, 67000
Abstract
Spontaneous generation of hierarchical order over multiple length scales remains a major challenge in soft materials because it typically relies on external patterning or multistep fabrication strategies. Here we show that a coacervate-like, exponentially growing poly(L-lysine)/hyaluronic acid (PLL/HA) multilayer autonomously reorganizes into a hierarchical architecture following simple exposure to ATP under aqueous conditions. Within minutes, the initially homogeneous film evolves into a sponge-like network of micrometer-sized cavities separated by thin walls containing PLL, HA and ATP. Cryogenic scanning electron microscopy and small-angle X-ray scattering independently reveal that these walls possess a short-range one-dimensional lamellar paracrystalline organization, demonstrating the emergence of structural order at both the micro- and nanoscales. The extent of this reorganization depends on the ATP concentration: 2 mM concentration of ATP produces a stable hierarchical morphology, whereas high ATP concentration drives complete film dissolution. Comparison with guanosine and uridine triphosphate (GTP and UTP) demonstrates that the self-organization process depends on the chemical nature of the nucleobase since, under exactly the same conditions, only ATP and GTP lead to a mesostructured formation. All our observations are consistent with a mechanistic framework in which a suitable nucleotide, i.e. ATP or GTP, progressively remodels the coacervate-like network, leading to an internal phase separation that may evolve into a lamellar structure through a surface-directed process. More broadly, this work identifies hydrated polyelectrolyte assemblies such as exponentially growing polyelectrolyte films, as a simple experimental platform in which diffusion-driven compositional changes can generate hierarchical periodic micro- and nanostructures without external templating.
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BibTeX
@misc{runser2026nucleotides,
title = {{Nucleotides trigger the spontaneous emergence of hierarchical nanolamellar architectures in coacervate-like polyelectrolyte multilayers}},
author = {Jean-Yves Runser and Shahaji H. More and Thierry Dintzer and Alain Carvalho and Marc Schmutz and Pierre Schaaf and Jérôme Combet and Loïc Jierry and Loïc JIERRY},
howpublished = {ChemRxiv},
year = {2026},
month = oct,
doi = {10.26434/chemrxiv.15011159/v1},
url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15011159/v1},
note = {CC BY},
}
RIS
TY - UNPB
TI - Nucleotides trigger the spontaneous emergence of hierarchical nanolamellar architectures in coacervate-like polyelectrolyte multilayers
AU - Jean-Yves Runser
AU - Shahaji H. More
AU - Thierry Dintzer
AU - Alain Carvalho
AU - Marc Schmutz
AU - Pierre Schaaf
AU - Jérôme Combet
AU - Loïc Jierry
AU - Loïc JIERRY
PY - 2026
DA - 2026/10/27
PB - ChemRxiv
DO - 10.26434/chemrxiv.15011159/v1
UR - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15011159/v1
AB - Spontaneous generation of hierarchical order over multiple length scales remains a major challenge in soft materials because it typically relies on external patterning or multistep fabrication strategies. Here we show that a coacervate-like, exponentially growing poly(L-lysine)/hyaluronic acid (PLL/HA) multilayer autonomously reorganizes into a hierarchical architecture following simple exposure to ATP under aqueous conditions. Within minutes, the initially homogeneous film evolves into a sponge-like network of micrometer-sized cavities separated by thin walls containing PLL, HA and ATP. Cryogenic scanning electron microscopy and small-angle X-ray scattering independently reveal that these walls possess a short-range one-dimensional lamellar paracrystalline organization, demonstrating the emergence of structural order at both the micro- and nanoscales. The extent of this reorganization depends on the ATP concentration: 2 mM concentration of ATP produces a stable hierarchical morphology, whereas high ATP concentration drives complete film dissolution. Comparison with guanosine and uridine triphosphate (GTP and UTP) demonstrates that the self-organization process depends on the chemical nature of the nucleobase since, under exactly the same conditions, only ATP and GTP lead to a mesostructured formation. All our observations are consistent with a mechanistic framework in which a suitable nucleotide, i.e. ATP or GTP, progressively remodels the coacervate-like network, leading to an internal phase separation that may evolve into a lamellar structure through a surface-directed process. More broadly, this work identifies hydrated polyelectrolyte assemblies such as exponentially growing polyelectrolyte films, as a simple experimental platform in which diffusion-driven compositional changes can generate hierarchical periodic micro- and nanostructures without external templating.
ER -