{
  "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.",
  "abstract_shown": true,
  "affiliations": [
    "Institut Charles Sadron (UPR22, 23 rue du Loess, Strasbourg Cedex, France, BP 84047",
    "CNRS, 25 rue Becquerel, Strasbourg Cedex, France, 67087",
    "CRBS, 1 rue Eugène Boeckel, Strasbourg, France, 67000",
    "Faculté de Chirurgie Dentaire, Université de Strasbourg, 8 rue Sainte Elisabeth, Strasbourg, France, 67000"
  ],
  "article_type": null,
  "arxiv": null,
  "author_total": 9,
  "authors": [
    {
      "affs": [
        0
      ],
      "name": "Jean-Yves Runser"
    },
    {
      "affs": [
        0
      ],
      "name": "Shahaji H. More"
    },
    {
      "affs": [
        1
      ],
      "name": "Thierry Dintzer"
    },
    {
      "affs": [
        0
      ],
      "name": "Alain Carvalho"
    },
    {
      "affs": [
        0
      ],
      "name": "Marc Schmutz"
    },
    {
      "affs": [
        2,
        3
      ],
      "name": "Pierre Schaaf"
    },
    {
      "affs": [
        0
      ],
      "name": "Jérôme Combet"
    },
    {
      "affs": [
        0
      ],
      "name": "Loïc Jierry"
    },
    {
      "name": "Loïc JIERRY",
      "orcid": "0000-0002-7541-1360"
    }
  ],
  "bibtex": "https://research.draconitic.com/paper/dwhgq0jak711q.bib",
  "cited_by": 0,
  "doi": "10.26434/chemrxiv.15011159/v1",
  "fulltext_url": null,
  "id": "dwhgq0jak711q",
  "issns": [],
  "landing_url": "https://chemrxiv.org/doi/full/10.26434/chemrxiv.15011159/v1",
  "language": null,
  "licence": "CC-BY",
  "licence_label": "CC BY",
  "licence_source": "journal",
  "licence_url": "https://creativecommons.org/licenses/by/4.0/",
  "metadata_licence": null,
  "native_subjects": [
    [
      "openalex",
      "2502|Supramolecular Self-Assembly in Materials"
    ]
  ],
  "openalex": "W7224135496",
  "pdf_url": "https://chemrxiv.org/doi/pdf/10.26434/chemrxiv.15011159/v1",
  "pmcid": null,
  "pmid": null,
  "published": "2026-10-27",
  "publisher": "American Chemical Society (ACS)",
  "ris": "https://research.draconitic.com/paper/dwhgq0jak711q.ris",
  "sources": [
    {
      "first_seen": "2026-10-30T12:17:26Z",
      "native_id": "10.26434/chemrxiv.15011159",
      "source": "chemrxiv",
      "url": "https://chemrxiv.org/doi/full/10.26434/chemrxiv.15011159/v1"
    }
  ],
  "subjects": [
    {
      "field": "chemistry",
      "origin": "openalex:2502|Supramolecular Self-Assembly in Materials",
      "subfield": "materials-polymers"
    }
  ],
  "title": "Nucleotides trigger the spontaneous emergence of hierarchical nanolamellar architectures in coacervate-like polyelectrolyte multilayers",
  "title_text": "Nucleotides trigger the spontaneous emergence of hierarchical nanolamellar architectures in coacervate-like polyelectrolyte multilayers",
  "type": "preprint",
  "updated_at": "2026-10-30T12:17:26Z",
  "url": "https://research.draconitic.com/paper/dwhgq0jak711q",
  "venue": "ChemRxiv",
  "versions": []
}