Most binary superlattices created using DNA functionalization or other approaches rely on particle size differences to achieve compositional order and structural diversity. Here we study two-dimensional (2D) assembly of DNAfunctionalized micron-sized particles (DFPs), and employ a strategy that leverages the tunable disparity in interparticle interactions, and thus enthalpic driving forces, to open new avenues for design of binary superlattices that do not rely on the ability to tune particle size (i.e., entropic driving forces). Our strategy employs tailored blends of complementary strands of ssDNA to control interparticle interactions between micron-sized silica particles in a binary mixture to create compositionally diverse 2D lattices. We show that the particle arrangement can be further controlled by changing the stoichiometry of the binary mixture in certain cases. With this approach, we demonstrate the ability to program the particle assembly into square, pentagonal, and hexagonal lattices. In addition, different particle types can be compositionally ordered in square checkerboard and hexagonal -alternating string, honeycomb, and Kagome arrangements. The field of DNA-mediated particle assembly has undergone remarkable progress over recent years (1), owing, at least in part, to its potential as a powerful platform for rational, bottomup design and engineering of complex materials, and motivated by recent successful translations into applications as diverse as sensing (2), photonics (3), and catalysis. The growing number of synthetic pathways and design strategies to fabricate DNA-functionalized particles (DFPs) has led to the development of a diverse palette of tailorable building blocks from which to choose, comprised of particles of a wide range of inorganic to organic compositions, a near continuum of particle sizes spanning nanometers to micrometers, precise DNA sequence control and thus tailorable hybridization, diverse chemistries for DNA grafting/association, and fine tunability of the grafting density. (4)(5)(6) Accompanying this expanding diversity of building blocks has been a parallel development of specific to generalized design principles that have begun to link molecular-scale DFP function with mechanisms of assembly and the resulting uni-or multi-modal crystalline structures.To this end, the growing combination of theory, simulations, and experiments, has helped to overcome some of the challenges in the field. For example, re-entrant melting strategies (7,8) have been successfully developed to alleviate the very narrow temperature ranges for efficient crystallization of DFPs.The most common route to induce attraction between DFPs, and thus program their assembly, leverages the direct or indirect (i.e., with additional DNA linker strand) hybridization of complementary DNA strands tethered separately to two types of particles. Under suitable conditions in such systems, particles with complementary DNA functionality (i.e., 'unlike' particles) form attractive contacts among multiple strands of h...
We systematically investigate the assembly of binary multi-flavored colloidal mixtures in two dimensions. In these mixtures all pairwise interactions between species may be tuned independently. This introduces an additional degree of freedom over more traditional binary mixtures with fixed mixing rules, which is anticipated to open new avenues for directed self-assembly. At present, colloidal self-assembly into non-trivial lattices tends to require either high pressures for isotropically interacting particles, or the introduction of directionally anisotropic interactions. Here we demonstrate tunable assembly into a plethora of structures which requires neither of these conditions. We develop a minimal model that defines a three-dimensional phase space containing one dimension for each pairwise interaction, then employ various computational techniques to map out regions of this phase space in which the system self-assembles into these different morphologies. We then present a mean-field model that is capable of reproducing these results for size-symmetric mixtures, which reveals how to target different structures by tuning pairwise interactions, solution stoichiometry, or both. Concerning particle size asymmetry, we find that domains in this model’s phase space, corresponding to different morphologies, tend to undergo a continuous “rotation” whose magnitude is proportional to the size asymmetry. Such continuity enables one to estimate the relative stability of different lattices for arbitrary size asymmetries. Owing to its simplicity and accuracy, we expect this model to serve as a valuable design tool for engineering binary colloidal crystals from multi-flavored components.
Binary superlattices constructed from nano- or micron-sized colloidal particles have a wide variety of applications, including the design of advanced materials. Self-assembly of such crystals from their constituent colloids can be achieved in practice by, among other means, the functionalization of colloid surfaces with single-stranded DNA sequences. However, when driven by DNA, this assembly is traditionally premised on the pairwise interaction between a single DNA sequence and its complement, and often relies on particle size asymmetry to entropically control the crystalline arrangement of its constituents. The recently proposed "multi-flavoring" motif for DNA functionalization, wherein multiple distinct strands of DNA are grafted in different ratios to different colloids, can be used to experimentally realize a binary mixture in which all pairwise interactions are independently controllable. In this work, we use various computational methods, including molecular dynamics and Wang-Landau Monte Carlo simulations, to study a multi-flavored binary system of micron-sized DNA-functionalized particles modeled implicitly by Fermi-Jagla pairwise interactions. We show how self-assembly of such systems can be controlled in a purely enthalpic manner, and by tuning only the interactions between like particles, demonstrate assembly into various morphologies. Although polymorphism is present over a wide range of pairwise interaction strengths, we show that careful selection of interactions can lead to the generation of pure compositionally ordered crystals. Additionally, we show how the crystal composition changes with the like-pair interaction strengths, and how the solution stoichiometry affects the assembled structures.
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