Hierarchical self-assembly for high-yield addressable complexity at fixed conditions

There is evidence that the self-assembly of complex molecular systems often proceeds hierarchically, by first building subunits that later assemble in larger entities, in a process that can repeat multiple times. Yet, our understanding of this phenomenon and its performance is limited. Here, we introduce a simple model for hierarchical addressable self-assembly, where interactions between particles can be optimized to maximize the fraction of a well-formed target structure, or yield. We find that a hierarchical strategy leads to an impressive yield up to at least five generations of the hierarchy and does not require a cycle of temperatures as used in previous methods. High yield is obtained when the microscopic interaction decreases with the scale of units considered, such that the total interaction between intermediate structures remains identical at all scales. We provide thermodynamic and dynamical arguments constraining the interaction strengths where this strategy is effective. Overall, our work characterizes an alternative strategy for addressable self-assembly at a fixed temperature, and provides insight into the mechanisms sustaining hierarchical assembly in biological systems.

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Publication Details

Journal
Proceedings of the National Academy of Sciences
Published
2025-10-22
DOI
https://doi.org/10.1073/pnas.2500245122
Citations
1
Primary Topic
Supramolecular Self-Assembly in Materials
Type
article
Field-Weighted Citation Impact
0.60
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article

Hierarchical self-assembly for high-yield addressable complexity at fixed conditions

Matthieu Wyart, Miranda Holmes‐Cerfon
1 citations
Proceedings of the National Academy of Sciences
Supramolecular Self-Assembly in Materials
0.60
article

Hierarchical self-assembly for high-yield addressable complexity at fixed conditions

Matthieu Wyart, Miranda Holmes‐Cerfon
article en
1 citations

Abstract

There is evidence that the self-assembly of complex molecular systems often proceeds hierarchically, by first building subunits that later assemble in larger entities, in a process that can repeat multiple times. Yet, our understanding of this phenomenon and its performance is limited. Here, we introduce a simple model for hierarchical addressable self-assembly, where interactions between particles can be optimized to maximize the fraction of a well-formed target structure, or yield. We find that a hierarchical strategy leads to an impressive yield up to at least five generations of the hierarchy and does not require a cycle of temperatures as used in previous methods. High yield is obtained when the microscopic interaction decreases with the scale of units considered, such that the total interaction between intermediate structures remains identical at all scales. We provide thermodynamic and dynamical arguments constraining the interaction strengths where this strategy is effective. Overall, our work characterizes an alternative strategy for addressable self-assembly at a fixed temperature, and provides insight into the mechanisms sustaining hierarchical assembly in biological systems.

Proceedings of the National Academy of SciencesVol. 122(43)
University of British Columbia (CA), Johns Hopkins University (US), FZU ‒ Institute of Physics of the Academy of Sciences of the Czech Republic (CZ), École Polytechnique Fédérale de Lausanne (CH), Toronto Metropolitan University (CA)
Openalex Percentile: Top 28%
Supramolecular Self-Assembly in Materials
0.60
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Hierarchical self-assembly for high-yield addressable complexity at fixed conditions — Matthieu Wyart, Miranda Holmes‐Cerfon · Proceedings of the National Academy of Sciences (2025) | TGRS Research Map | TGRS