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Designing the ground state is not enough: Lessons from the self-assembly of Archimedean shells
Luigi Graziano1, Niccolò Tedeschi2, Petr Šulc2,3
1Dipartimento di Fisica, Sapienza Università di Roma, P.le Aldo Moro 5, 00185 Rome, Italy.
The Journal of Chemical Physics
|July 22, 2026
Summary
Entropy can favor incorrect structures in particle self-assembly, even when the target is energetically optimal. Accounting for entropy and bond flexibility is crucial for successful inverse design strategies.
Area of Science:
- Colloidal self-assembly
- Thermodynamics
- Materials science
Background:
- Designing self-assembling particles to form a specific target structure requires it to be the thermodynamic ground state.
- However, achieving successful assembly at finite temperatures is challenging, as competing structures can emerge due to entropic effects.
Purpose of the Study:
- To investigate the influence of entropic contributions on the thermodynamic stability of competing aggregates in colloidal self-assembly.
- To provide quantitative guidelines for inverse design strategies that consider entropy and bond flexibility.
Main Methods:
- Utilized a cluster-based thermodynamic approach to compute the free-energy landscape of competing aggregates.
- Focused on the colloidal Archimedean snub-cube as a model system.
Main Results:
- The target structure was uniquely selected at the potential energy level.
- Entropic contributions favored competing clusters, particularly with high bond directionality.
- Incomplete structures like icosahedra were stabilized entropically, despite higher energy, suppressing target yield.
Conclusions:
- Potential energy alone is insufficient to guarantee successful self-assembly at finite temperatures.
- Entropy plays a critical role, potentially stabilizing undesired structures.
- Inverse design strategies must explicitly incorporate entropy, bond flexibility, and experimental conditions for improved yield.
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