ArticleProceedings of the National Academy of Sciences of the United States of America2022
A theory of entropic bonding.
Article in Proceedings of the National Academy of Sciences of the United States of America, 2022. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 8 papers.
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Who cites it
8 citing papers in PubMed.
- Tunable Plasmonic Circular Dichroism of Hierarchical Chiral Assemblies.Chemistry of materials : a publication of the American Chemical Society · 2025Article
- Encoding hierarchical 3D architecture through inverse design of programmable bonds.Nature materials · 2025Article
- Superstructural phase transitions in polymer-grafted nanooctahedra.Science advances · 2025Article
- Article
- Self-assembled soft alloy with Frank-Kasper phases beyond metals.Nature materials · 2024Article
- Quantum-inspired encoding enhances stochastic sampling of soft matter systems.Science advances · 2023Article
- Entropy compartmentalization stabilizes open host-guest colloidal clathrates.Nature chemistry · 2023Article
- Entropically engineered formation of fivefold and icosahedral twinned clusters of colloidal shapes.Nature communications · 2022Article
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2 authors.
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Abstract
Entropy alone can self-assemble hard nanoparticles into colloidal crystals of remarkable complexity whose structures are the same as atomic and molecular crystals, but with larger lattice spacings. Molecular simulation is a powerful tool used extensively to study the self-assembly of ordered phases from disordered fluid phases of atoms, molecules, or nanoparticles. However, it is not yet possible to predict colloidal crystal structures a priori from particle shape as we can for atomic crystals from electronic valency. Here, we present such a first-principles theory. By calculating and minimizing excluded volume within the framework of statistical mechanics, we describe the directional entropic forces that collectively emerge between hard shapes, in familiar terms used to describe chemical bonds. We validate our theory by demonstrating that it predicts thermodynamically preferred structures for four families of hard polyhedra that match, in every instance, previous simulation results. The success of this first-principles approach to entropic colloidal crystal structure prediction furthers fundamental understanding of both entropically driven crystallization and conceptual pictures of bonding in matter.
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