Programming patchy particles for materials assembly design

Proceedings of the National Academy of Sciences, Journal Year: 2024, Volume and Issue: 121(27)

Published: June 24, 2024

Direct design of complex functional materials would revolutionize technologies ranging from printable organs to novel clean energy devices. However, even incremental steps toward designing have proven challenging. If the material is constructed highly components, space properties rapidly becomes too computationally expensive search. On other hand, very simple components such as uniform spherical particles are not powerful enough capture rich behavior. Here, we introduce a differentiable model with that yet properties: rigid bodies composed directional interactions (patchy particles). We showcase method self-assembly designs open lattices self-limiting clusters, all which notoriously challenging goals achieve using purely isotropic particles. By directly optimizing over location and interaction patches on patchy gradient descent, dramatically reduce computation time for finding optimal building blocks.

Language: Английский

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Limits of economy and fidelity for programmable assembly of size-controlled triply periodic polyhedra

Proceedings of the National Academy of Sciences, Journal Year: 2024, Volume and Issue: 121(18)

Published: April 26, 2024

We propose and investigate an extension of the Caspar-Klug symmetry principles for viral capsid assembly to programmable size-controlled triply periodic polyhedra, discrete variants Primitive, Diamond, Gyroid cubic minimal surfaces. Inspired by a recent class DNA origami colloids, we demonstrate that economy design in these crystalline assemblies-in terms growth number distinct particle species required with increased size-scale (e.g., periodicity)-is comparable shells. further test role geometric specificity assemblies via dynamical simulations, which show conditions simultaneously efficient high-fidelity require intermediate degree flexibility local angles lengths programmed assembly. Off-target misassembly occurs incorporation variant disclination defects, generalized case hyperbolic crystals. The possibility topological defects is direct consequence very same underlie economical design, exposing basic tradeoff between fidelity programmable, size controlled

Language: Английский

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Economical routes to size-specific assembly of self-closing structures

Science Advances, Journal Year: 2024, Volume and Issue: 10(27)

Published: July 3, 2024

Programmable self-assembly has seen an explosion in the diversity of synthetic crystalline materials, but developing strategies that target "self-limiting" assemblies remained a challenge. Among these, self-closing structures, which local curvature defines finite global size, are prone to polymorphism due thermal bending fluctuations, problem worsens with increasing size. Here, we show assembly complexity can be used eliminate this source tubules. Using many distinct components, prune density off-target geometries, selectivity tubule width and helicity nearly 100%. We further by reducing design constraints either pitch or alone, fewer components needed reach complete selectivity. Combining experiments theory, reveal economical limit, determines minimum number required create arbitrary sizes full

Language: Английский

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Vesicle shape transformations driven by confined active filaments

Nature Communications, Journal Year: 2021, Volume and Issue: 12(1)

Published: Dec. 13, 2021

In active matter systems, deformable boundaries provide a mechanism to organize internal stresses. To study minimal model of such system, we perform particle-based simulations an elastic vesicle containing collection polar filaments. The interplay between the stress organization due interparticle interactions and that deformability confinement leads variety filament spatiotemporal organizations have not been observed in bulk systems or under rigid confinement, including highly-aligned rings caps. turn, these assemblies drive dramatic tunable transformations shape its dynamics. We present simple scaling models reveal mechanisms underlying emergent behaviors yield design principles for engineering materials with targeted

Language: Английский

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Mechanisms of Scaffold-Mediated Microcompartment Assembly and Size Control

ACS Nano, Journal Year: 2021, Volume and Issue: 15(3), P. 4197 - 4212

Published: March 8, 2021

This article describes a theoretical and computational study of the dynamical assembly protein shell around complex consisting many cargo molecules long, flexible scaffold molecules. Our is motivated by bacterial microcompartments, which are proteinaceous organelles that assemble condensed droplet enzymes reactants. As in examples cytoplasmic liquid–liquid phase separation, condensation microcompartment interior driven proteins have weak multivalent interactions with cargo. results predict size, amount encapsulated cargo, pathways depend sensitively on properties scaffold, including its length valency scaffold–cargo interactions. Moreover, ability self-assembling shells to change their size accommodate different lengths depends crucially whether spontaneous curvature radius smaller or larger than characteristic elastic scale shell. Beyond natural these important implications for synthetic biology efforts target alternative encapsulation microcompartments viral shells. More broadly, elucidate how cells exploit coupling between self-assembly separation organize interiors.

Language: Английский

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Virus Assembly Pathways Inside a Host Cell

ACS Nano, Journal Year: 2022, Volume and Issue: 16(1), P. 317 - 327

Published: Jan. 12, 2022

Simple RNA viruses self-assemble spontaneously and encapsulate their genome into a shell called the capsid. This process is mainly driven by attractive electrostatics interaction between positive charges on capsid proteins negative genome. Despite its importance many decades of intense research, how virus selects packages native inside crowded environment host cell cytoplasm in presence an abundance nonviral other anionic polymers has remained mystery. In this paper, we perform series simulations to monitor growth viral shells find mechanism which cargo–coat protein interactions can impact structure stability shells. We show that coat subunits assemble around globular nucleic acid core forming nonicosahedral cages, have been recently observed assembly experiments involving small pieces RNA. resulting cages are strained easily be split fragments along stress lines. suggests such metastable intermediates could reassembled stable icosahedral if larger wild-type becomes available, despite myriad RNAs.

Language: Английский

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Anti‐cooperative Self‐Assembly with Maintained Emission Regulated by Conformational and Steric Effects

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(17)

Published: Feb. 3, 2022

Herein, we present a strategy to enable maintained emissive behavior in the self-assembled state by enforcing an anti-cooperative self-assembly involving weak intermolecular dye interactions. To achieve this goal, designed conformationally flexible monomer unit 1 with central 1,3-substituted (diphenyl)urea hydrogen bonding synthon that is tethered two BODIPY dyes featuring sterically bulky trialkoxybenzene substituents at meso-position. The competition between attractive forces (H-bonding and aromatic interactions) destabilizing effects (steric competing conformational effects) limits assembly, halting supramolecular growth stage of small oligomers. Given presence dye-dye interactions, emission properties molecularly dissolved are negligibly affected upon aggregation. Our findings contribute broadening scope assemblies controlled polymerization.

Language: Английский

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Thermodynamic Size Control in Curvature-Frustrated Tubules: Self-Limitation with Open Boundaries

ACS Nano, Journal Year: 2022, Volume and Issue: 16(6), P. 9077 - 9085

Published: May 31, 2022

We use computational modeling to investigate the assembly thermodynamics of a particle-based model for geometrically frustrated assembly, in which local packing geometry subunits is incompatible with uniform, strain-free large-scale assembly. The considers discrete triangular that drive toward closed, hexagonal-ordered tubule, but have geometries locally favor negative Gaussian curvature. dynamical Monte Carlo simulations and enhanced sampling methods compute free energy landscape corresponding self-assembly behavior as function experimentally accessible parameters control driving forces magnitude frustration. results determine parameter range where finite-temperature self-limiting occurs, equilibrium size distribution sharply peaked around well-defined finite size. also identify two mechanisms by system can escape frustration assemble unlimited size, particle-scale properties suppress unbounded growth.

Language: Английский

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Genetically Engineered, Multichromophore Virus-Like Nanoparticles with Ultranarrow Distribution of Emission Intensity

ACS Nano, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 3, 2025

Variance in the properties of optical mesoscopic probes is often a limiting factor applications. In thermodynamic limit, smaller probe, larger relative variance. However, specific viral protein cages can assemble efficiently outside bounds statistical fluctuations at equilibrium through process that characterized by intrinsic quality-control and self-limiting capabilities. this paper, an approach described leverages stoichiometric structural accuracy murine polyoma virus capsid assembly to demonstrate bright, narrowly distributed fluorescence intensity from multichromophore particles surpass state-of-the-art fluorescent nanosphere probes. Charge-detection mass spectrometry analysis demonstrated proteins resulting fusion superfolding green (sfGFP) coat self-assemble

Language: Английский

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Colloidal Crystallization on Cones

Physical Review Letters, Journal Year: 2025, Volume and Issue: 134(1)

Published: Jan. 3, 2025

We explore experimentally how a conical surface frustrates the growth of colloidal crystals. Whereas crystals on cylinder can form perfect commensurate bands, cone tend to tilt grain boundaries with misorientation angles set by geometry. However, at small angles, where deviates only slightly from that cylinder, widths limited emergence dislocations. The dislocations allow crystal continue growing beyond limiting width. relate these effects gradient in circumference cone, consequence Gaussian curvature localized apex.

Language: Английский

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