Self-limiting stacks of curvature-frustrated colloidal plates: Roles of intraparticle versus interparticle deformations DOI
Kyle T. Sullivan, Ryan C. Hayward, Gregory M. Grason

et al.

Physical review. E, Journal Year: 2024, Volume and Issue: 110(2)

Published: Aug. 9, 2024

In geometrically frustrated assemblies local intersubunit misfits propagate to intra-assembly strain gradients, giving rise anomalous self-limiting assembly thermodynamics. Here we use theory and coarse-grained simulation study a recently developed class of "curvamer" particles, flexible shell-like particles that exhibit due the build up curvature deformation in cohesive stacks. To address generic, yet poorly understood aspect assembly, introduce model curvamer incorporates both intraparticle shape as well compliance interparticle gaps, an effect can attribute finite range attraction between particles. We show ratio (bending elasticity) stiffness not only controls regimes self-limitation but also nature frustration propagation through find transition from uniformly bound, curvature-focusing stacks at small size gap opened, curved large is controlled by dimensionless measure inter- versus intracurvamer stiffness. The determines cohesion are self-limiting, prediction which strong agreement with numerical studies our colloidal model. These predictions provide critical guidance for experimental realizations particle systems designed especially multiparticle scales.

Language: Английский

Symmetry-Guided Inverse Design of Self-Assembling Multiscale DNA Origami Tilings DOI
Daichi Hayakawa, Thomas E. Videbæk, Gregory M. Grason

et al.

ACS Nano, Journal Year: 2024, Volume and Issue: 18(29), P. 19169 - 19178

Published: July 9, 2024

Recent advances enable the creation of nanoscale building blocks with complex geometries and interaction specificities for self-assembly. This nearly boundless design space necessitates principles defining mutual interactions between multiple particle species to target a user-specified structure or pattern. In this article, we develop symmetry-based method generate matrices that specify assembly two-dimensional tilings, which illustrate using equilateral triangles. By exploiting allowed 2D symmetries, an algorithmic approach by any periodic tiling can be generated from arbitrarily large number subunit species, notably addressing unmet challenge engineering crystals periodicities larger than size. To demonstrate utility our approach, encode specific triangular subunits synthesized DNA origami show guide their self-assembly into tilings wide variety up 12 unique conjugating triangles gold nanoparticles, fabricate gold-nanoparticle supracrystals whose lattice parameter spans 300 nm. Finally, economical rules, compare economy various tilings. particular, (1) higher symmetries allow unit cells fewer (2) linear designed more economically primitive cells. work provides simple designing assemblies, aiding in multiscale nanostructured "meta-atoms" engineered plasmonic functions.

Language: Английский

Citations

10
Accessing Semiaddressable Self-Assembly with Efficient Structure Enumeration DOI

Maximilian C. Hübl,

Carl P. Goodrich

Physical Review Letters, Journal Year: 2025, Volume and Issue: 134(5)

Published: Feb. 7, 2025

Modern experimental methods enable the creation of self-assembly building blocks with tunable interactions, but optimally exploiting this tunability for desired structures remains an important challenge. Many studies inverse problem start so-called fully addressable limit, where every particle in a target structure is different. This leads to clear design principles that often result high assembly yield, it not scalable approach-at some point, one must grapple "reusing" blocks, which lowers degree addressability and may cause multitude off-target form, complicating process. Here, we solve key obstacle preventing robust "semiaddressable regime" by developing highly efficient algorithm enumerates all can be formed from given set blocks. By combining established partition-function-based yield calculations, show almost always possible find economical semiaddressable designs entropic gain reusing outweighs presence even increases target. Thus, only does our enumeration regime, results demonstrate operate regime while maintaining level control associated full addressability.

Language: Английский

Citations

0
Arbitrary Design of DNA-Programmable 3D Crystals through Symmetry Mapping DOI Creative Commons
Jason S. Kahn, Daniel C. Redeker, Aaron Michelson

et al.

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

Published: April 11, 2025

Nanoscale self-assembly offers exciting potential for creating intricate structures beyond the limits of traditional top-down nanofabrication. Despite advancements in molecularly programmable assembly, particularly utilizing DNA nanotechnology, challenges remain defining precise assembly instructions formation complex three-dimensional (3D) superlattice architectures. DNA-based methods offer programmability through sequence-encoded addressable bonds, but difficulty lies reducing complexity and number these interactions to establish a modular, structural design strategy streamline component fabrication process. This work proposes symmetry-mapping bond assignment algorithm guide arbitrarily prescribed 3D lattices self-assembled from voxels with directional, bonds capable carrying nanocargo. The enables minimization voxels, thus amount information required encode assembly. developed approach leverages symmetries target lattices, assembled significantly incorporates experimentally relevant binding rules restrictions specific systems. We discuss demonstrate its capability selected examples nanoscale analogs zinc blende (ZnS) cubic Laves phase (MgCu2), as well lattice based on an designed motif (letter H). Through established associated software Mapping Of Structurally Encoded aSsembly (MOSES), this inverse provides scalable solution designing complexly organized nanostructures, providing means programming bottom-up nanomaterial fabrication.

Language: Английский

Citations

0
Chiral Self‐Assembly of Biphenyl‐Cored Carbohydrate Bolaamphiphiles and Molecular Dynamic Simulation‐Derived Mechanistic Insights DOI

Kingshuk Bag,

Dibyendu Mondal, Govardhan Reddy

et al.

Small, Journal Year: 2025, Volume and Issue: unknown

Published: April 27, 2025

Abstract The presence of multiple chiral centers and constitutions in carbohydrates opens up a facile access to uncover supramolecular chirality properties self‐assembled carbohydrate bolaamphiphiles. In this work, bolaamphiphiles are presented that present monosaccharide moieties at the termini an internal p , ′‐biphenyl core segment. segment exhibits planar twisting, which promotes self‐assembly α‐D‐Mannopyranoside‐biphenyl‐mannopyranoside bolaamphiphile self‐assembles with helicity, whereas α‐L‐rhamnopyranoside‐biphenyl‐rhamnopyranoside inverts helicity aq. solutions. propensity for emerging depends on pH solution, where alkaline retains acidic abolishes same. concentration dependence is evaluated solution. Molecular dynamics (MD) simulation studies reveal thermodynamic states interactions crucial biphenyl correlated terphenyl Morphological by microscopies ascertain helicities solid state. multivalent presentation α‐D‐mannopyranoside structures permits complexation relevant lectin, as assessed turbidity assays. Cytotoxicity assessments MCF‐7 cell line α‐L‐rhamnopyranoside has IC 50 89.6 ± 3.3 µ m indicating higher toxicity compared bolaamphiphile, greater than 100 .

Language: Английский

Citations

0
DNA Origami Colloidal Crystals: Opportunities and Challenges DOI
Jaewon Lee, Jangwon Kim, Gregor Posnjak

et al.

Nano Letters, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 20, 2024

Over the last three decades, colloidal crystallization has provided an easy-to-craft platform for mesoscale engineering of photonic and phononic crystals. Nevertheless, crystal lattices achieved thus far with commodity colloids are largely limited to symmetric densely packed structures, restricting their functionalities. To obtain non-close-packed crystals resulting complexity available directional binding between "patchy" been pursued. However, conventional have restricted micrometer-scale spherical particles or clusters. In this Mini-Review, we argue that time come widen scope palette include made using DNA origami. By benefiting from its unprecedented ability control nanoscale shapes patch placement incorporate various nanomaterials, origami enables novel crystallization, particularly applications. This mini-review summarizes recent progress on together challenges opportunities.

Language: Английский

Citations

2
Automating Blueprints for the Assembly of Colloidal Quasicrystal Clusters DOI
Diogo E. P. Pinto, Petr Šulc, Francesco Sciortino

et al.

ACS Nano, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 20, 2024

One of the frontiers nanotechnology is advancing beyond periodic self-assembly materials. Icosahedral quasicrystals, aperiodic in all directions, represent one most challenging targets that has yet to be experimentally realized at colloidal scale. Previous attempts have required meticulous human-designed building blocks and often resulted interactions current experimental capabilities. In this work, we introduce a framework for generating accessible designs self-assemble into quasicrystalline arrangements. We present design icosahedral deoxyribonucleic acid (DNA) origami demonstrate, through molecular simulations, their successful assembly target structure. Our results highlight feasibility using automated protocols achieve complex patterns, with applications material science nanotechnology.

Language: Английский

Citations

1
Self-limiting stacks of curvature-frustrated colloidal plates: Roles of intraparticle versus interparticle deformations DOI
Kyle T. Sullivan, Ryan C. Hayward, Gregory M. Grason

et al.

Physical review. E, Journal Year: 2024, Volume and Issue: 110(2)

Published: Aug. 9, 2024

In geometrically frustrated assemblies local intersubunit misfits propagate to intra-assembly strain gradients, giving rise anomalous self-limiting assembly thermodynamics. Here we use theory and coarse-grained simulation study a recently developed class of "curvamer" particles, flexible shell-like particles that exhibit due the build up curvature deformation in cohesive stacks. To address generic, yet poorly understood aspect assembly, introduce model curvamer incorporates both intraparticle shape as well compliance interparticle gaps, an effect can attribute finite range attraction between particles. We show ratio (bending elasticity) stiffness not only controls regimes self-limitation but also nature frustration propagation through find transition from uniformly bound, curvature-focusing stacks at small size gap opened, curved large is controlled by dimensionless measure inter- versus intracurvamer stiffness. The determines cohesion are self-limiting, prediction which strong agreement with numerical studies our colloidal model. These predictions provide critical guidance for experimental realizations particle systems designed especially multiparticle scales.

Language: Английский

Citations

0