Magic sizes enable minimal-complexity, high-fidelity assembly of programmable shells

Fuente: arXiv
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Auteurs principaux: Tyukodi, Botond, Caballero, Fernando, Hayakawa, Daichi, Hall, Douglas M., Rogers, W. Benjamin, Grason, Gregory M., Hagan, Michael F.
Format: Preprint
Publié: 2024
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author Tyukodi, Botond
Caballero, Fernando
Hayakawa, Daichi
Hall, Douglas M.
Rogers, W. Benjamin
Grason, Gregory M.
Hagan, Michael F.
author_facet Tyukodi, Botond
Caballero, Fernando
Hayakawa, Daichi
Hall, Douglas M.
Rogers, W. Benjamin
Grason, Gregory M.
Hagan, Michael F.
contents Recent advances in synthetic methods enable designing subunits that self-assemble into structures with precise, finite sizes and well-defined architectures, but yields are frequently suppressed by the formation of off-target metastable structures. Increasing the complexity (the number of distinct subunit types) can inhibit off-target structures, but leads to slower kinetics and higher synthesis costs. Here, we study icosahedral shells formed of programmable triangular subunits as a model system, and identify design principles that produce the highest target yield at the lowest complexity. We use a symmetry-based construction to create a range of design complexities, starting from the maximal symmetry Caspar-Klug assembly up to the fully addressable, zero-symmetry assembly. Kinetic Monte Carlo simulations reveal that the most prominent defects leading to off-target assemblies are disclinations at sites of rotational symmetry. We derive symmetry-based rules for identifying the optimal (lowest-complexity, highest-symmetry) design that inhibits these disclinations, leading to robust, high-fidelity assembly of targets with arbitrarily large, yet precise, finite sizes. The optimal complexity varies non-monotonically with target size, with `magic' sizes appearing for high-symmetry designs in which symmetry axes do not intersect vertices of the triangular net. The optimal designs at magic sizes require 12 times fewer inequivalent interaction-types than the (minimal symmetry) fully addressable construction, which greatly reduces the timescale and experimental cost required to achieve high fidelity assembly of large targets. This symmetry-based principle for pruning off-target assembly generalizes to diverse architectures with different topologies.
format Preprint
id arxiv_https___arxiv_org_abs_2411_03720
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Magic sizes enable minimal-complexity, high-fidelity assembly of programmable shells
Tyukodi, Botond
Caballero, Fernando
Hayakawa, Daichi
Hall, Douglas M.
Rogers, W. Benjamin
Grason, Gregory M.
Hagan, Michael F.
Soft Condensed Matter
Recent advances in synthetic methods enable designing subunits that self-assemble into structures with precise, finite sizes and well-defined architectures, but yields are frequently suppressed by the formation of off-target metastable structures. Increasing the complexity (the number of distinct subunit types) can inhibit off-target structures, but leads to slower kinetics and higher synthesis costs. Here, we study icosahedral shells formed of programmable triangular subunits as a model system, and identify design principles that produce the highest target yield at the lowest complexity. We use a symmetry-based construction to create a range of design complexities, starting from the maximal symmetry Caspar-Klug assembly up to the fully addressable, zero-symmetry assembly. Kinetic Monte Carlo simulations reveal that the most prominent defects leading to off-target assemblies are disclinations at sites of rotational symmetry. We derive symmetry-based rules for identifying the optimal (lowest-complexity, highest-symmetry) design that inhibits these disclinations, leading to robust, high-fidelity assembly of targets with arbitrarily large, yet precise, finite sizes. The optimal complexity varies non-monotonically with target size, with `magic' sizes appearing for high-symmetry designs in which symmetry axes do not intersect vertices of the triangular net. The optimal designs at magic sizes require 12 times fewer inequivalent interaction-types than the (minimal symmetry) fully addressable construction, which greatly reduces the timescale and experimental cost required to achieve high fidelity assembly of large targets. This symmetry-based principle for pruning off-target assembly generalizes to diverse architectures with different topologies.
title Magic sizes enable minimal-complexity, high-fidelity assembly of programmable shells
topic Soft Condensed Matter
url https://arxiv.org/abs/2411.03720