2018/12/19 by Pritam Kumar Jana, Bortolo Matteo Mognetti · 11 citations
Biochemistry, Genetics and Molecular Biology · Chemistry · Materials Science · Physics and Astronomy · #Advanced biosensing and bioanalysis techniques #Cascade #Chemical engineering #Chemical physics #Chemistry #Colloid #Colloidal crystal #Colloidal particle #Crystallography #DNA #Geometry #Gold and Silver Nanoparticles Synthesis and Applications #Materials science #Nanotechnology #Polymer Surface Interaction Studies #Self-assembly #Surface (topology) #Surface modification #cond-mat.soft #physics.bio-ph
paper · pdf · doi:10.1039/c8nr10217a
published in Nanoscale 11(12), 5450-5459 (Royal Society of Chemistry)
arxiv created 2018/12/19 · openalex publication_date 2019/01/01 · arxiv updated 2019/02/26 · openalex created_date 2025/10/10 · openalex updated_date 2026/08/05
Functionalizing colloids with reactive DNA linkers is a versatile way of programming self-assembly. DNA selectivity provides direct control over colloid-colloid interactions allowing the engineering of structures such as complex crystals or gels. However, the self-assembly of localized and finite structures remains an open problem with many potential applications. In this work, we present a system in which functionalized surfaces initiate a cascade reaction between linkers leading to the self-assembly of crystals with a controllable number of layers. Specifically, we consider colloidal particles functionalized by two families of complementary DNA linkers with mobile anchoring points, as found in experiments using emulsions or lipid bilayers. In bulk, intra-particle linkages formed by pairs of complementary linkers prevent the formation of inter-particle bridges and therefore colloid-colloid aggregation. However, colloids interact strongly with the surface given that the latter can destabilize intra-particle linkages. When in direct contact with the surface, colloids are activated, meaning that they feature more unpaired DNA linkers ready to react. Activated colloids can then capture and activate other colloids from the bulk through the formation of inter-particle linkages. Using simulations and theory, validated by existing experiments, we clarify the thermodynamics of the activation and binding process and explain how particle-particle interactions, within the adsorbed phase, weaken as a function of the distance from the surface. The latter observation underlies the possibility of self-assembling finite aggregates with controllable thickness and flat solid-gas interfaces. Our design suggests a new avenue to fabricate heterogeneous and finite structures.