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1. Directing and reconfiguring colloidal assembly by disclination networks in nematic liquid crystal as templates

   https://doi.org/10.1016/j.giant.2023.100228  

   Guo, Yubing ; Jiang, Miao ; Afghah, Sajedeh ; Peng, Chenghui ; Selinger, Robin LB ; Lavrentovich, Oleg D ; Wei, Qi-Huo ( March 2024 , Giant)

   Exotic structures with interesting physical and chemical properties can be achieved by self-organizing engineered building blocks. The central aim for self-assembly is to precisely control the position and orientation of individual building blocks. In this work, we use topological defects (disclinations) in nematic liquid crystals as templates to direct the self-assembly of colloidal particles into designable 3D structures. By photopatterning preprogrammed molecular orientations at two confining surfaces, we created pre-designable disclination networks and characterized their interactions with spherical colloidal particles. We find that colloidal particles are attracted to different disclinations depending on the orientation of the point defect (elastic dipole) around the colloids. We demonstrate that the positions, network structures, and orientation of the elastic dipoles of the colloidal chains can be pre-designed and reconfigured with remote illumination of polarized light. 

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2. Repulsion–attraction switching of nematic colloids formed by liquid crystal dispersions of polygonal prisms

   https://doi.org/10.1039/c7sm01186e  

   Senyuk, B. ; Liu, Q. ; Nystrom, P. D. ; Smalyukh, I. I. ( January 2017 , Soft Matter)

   Self-assembly of colloidal particles due to elastic interactions in nematic liquid crystals promises tunable composite materials and can be guided by exploiting surface functionalization, geometric shape and topology, though these means of controlling self-assembly remain limited. Here, we realize low-symmetry achiral and chiral elastic colloids in the nematic liquid crystals using colloidal polygonal concave and convex prisms. We show that the controlled pinning of disclinations at the prism edges alters the symmetry of director distortions around the prisms and their orientation with respect to the far-field director. The controlled localization of the disclinations at the prism's edges significantly influences the anisotropy of the diffusion properties of prisms dispersed in liquid crystals and allows one to modify their self-assembly. We show that elastic interactions between polygonal prisms can be switched between repulsive and attractive just by controlled re-pinning the disclinations at different edges using laser tweezers. Our findings demonstrate that elastic interactions between colloidal particles dispersed in nematic liquid crystals are sensitive to the topologically equivalent but geometrically rich controlled configurations of the particle-induced defects. 

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3. Building blocks of non-Euclidean ribbons: size-controlled self-assembly via discrete frustrated particles

   https://doi.org/10.1039/D2SM01371A  

   Hall, Douglas M. ; Stevens, Mark J. ; Grason, Gregory M. ( February 2023 , Soft Matter)

   Geometric frustration offers a pathway to soft matter self-assembly with controllable finite sizes. While the understanding of frustration in soft matter assembly derives almost exclusively from continuum elastic descriptions, a current challenge is to understand the connection between microscopic physical properties of misfitting “building blocks” and emergent assembly behavior at the mesoscale. We present and analyze a particle-based description of what is arguably the best studied example for frustrated soft matter assembly, negative-curvature ribbon assembly, observed in both assemblies of chiral surfactants and shape-frustrated nanoparticles. Based on our particle model, known as saddle wedge monomers, we numerically test the connection between microscopic shape and interactions of the misfitting subunits and the emergent behavior at the supra-particle scale, specifically focussing on the propagation and relaxation of inter-particle strains, the emergent role of extrinsic shape on frustrated ribbons and the equilibrium regime of finite width selection. Beyond the intuitive role of shape misfit, we show that self-limitation is critically dependent on the finite range of cohesive interactions, with larger size finite assemblies requiring increasing short-range interparticle forces. Additionally, we demonstrate that non-linearities arising from discrete particle interactions alter self-limiting behavior due to both strain-softening in shape-flattened assembly and partial yielding of highly strained bonds, which in turn may give rise to states of hierarchical, multidomain assembly. Tracing the regimes of frustration-limited assembly to the specific microscopic features of misfitting particle shapes and interactions provides necessary guidance for translating the theory of size-programmable assembly into design of intentionally-frustrated colloidal particles. 

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4. A computational toolbox for the assembly yield of complex and heterogeneous structures

   https://doi.org/10.1038/s41467-023-43168-4  

   Curatolo, Agnese I. ; Kimchi, Ofer ; Goodrich, Carl P. ; Krueger, Ryan K. ; Brenner, Michael P. ( December 2023 , Nature Communications)

   The self-assembly of complex structures from a set of non-identical building blocks is a hallmark of soft matter and biological systems, including protein complexes, colloidal clusters, and DNA-based assemblies. Predicting the dependence of the equilibrium assembly yield on the concentrations and interaction energies of building blocks is highly challenging, owing to the difficulty of computing the entropic contributions to the free energy of the many structures that compete with the ground state configuration. While these calculations yield well known results for spherically symmetric building blocks, they do not hold when the building blocks have internal rotational degrees of freedom. Here we present an approach for solving this problem that works with arbitrary building blocks, including proteins with known structure and complex colloidal building blocks. Our algorithm combines classical statistical mechanics with recently developed computational tools for automatic differentiation. Automatic differentiation allows efficient evaluation of equilibrium averages over configurations that would otherwise be intractable. We demonstrate the validity of our framework by comparison to molecular dynamics simulations of simple examples, and apply it to calculate the yield curves for known protein complexes and for the assembly of colloidal shells.

    

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5. Programming interactions in magnetic handshake materials

   https://doi.org/10.1039/D2SM00604A  

   Du, Chrisy Xiyu ; Zhang, Hanyu Alice ; Pearson, Tanner G. ; Ng, Jakin ; McEuen, Paul L. ; Cohen, Itai ; Brenner, Michael P. ( August 2022 , Soft Matter)

   The ability to rapidly manufacture building blocks with specific binding interactions is a key aspect of programmable assembly. Recent developments in DNA nanotechnology and colloidal particle synthesis have significantly advanced our ability to create particle sets with programmable interactions, based on DNA or shape complementarity. The increasing miniaturization underlying magnetic storage offers a new path for engineering programmable components for self assembly, by printing magnetic dipole patterns on substrates using nanotechnology. How to efficiently design dipole patterns for programmable assembly remains an open question as the design space is combinatorially large. Here, we present design rules for programming these magnetic interactions. By optimizing the structure of the dipole pattern, we demonstrate that the number of independent building blocks scales super linearly with the number of printed domains. We test these design rules using computational simulations of self assembled blocks, and experimental realizations of the blocks at the mm scale, demonstrating that the designed blocks give high yield assembly. In addition, our design rules indicate that with current printing technology, micron sized magnetic panels could easily achieve hundreds of different building blocks. 

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