Publications

2013
Schade NB, Holmes-Cerfon MC, Chen ER, Aronzon D, Collins JW, Fan JA, Capasso F, Manoharan VN. Tetrahedral Colloidal Clusters from Random Parking of Bidisperse Spheres. Physical Review Letters. 2013;110 :148303. Publisher's VersionAbstract
Using experiments and simulations, we investigate the clusters that form when colloidal spheres stick irreversibly to—or “park” on—smaller spheres. We use either oppositely charged particles or particles labeled with complementary DNA sequences, and we vary the ratio α of large to small sphere radii. Once bound, the large spheres cannot rearrange, and thus the clusters do not form dense or symmetric packings. Nevertheless, this stochastic aggregation process yields a remarkably narrow distribution of clusters with nearly 90% tetrahedra at α=2.45. The high yield of tetrahedra, which reaches 100% in simulations at α=2.41, arises not simply because of packing constraints, but also because of the existence of a long-time lower bound that we call the “minimum parking” number. We derive this lower bound from solutions to the classic mathematical problem of spherical covering, and we show that there is a critical size ratio αc=(1+√2)≈2.41, close to the observed point of maximum yield, where the lower bound equals the upper bound set by packing constraints. The emergence of a critical value in a random aggregation process offers a robust method to assemble uniform clusters for a variety of applications, including metamaterials.
Lee Y-J, Schade NB, Sun L, Fan JA, Bae DR, Mariscal MM, Lee G, Capasso F, Sacanna S, Manoharan VN, et al. Ultrasmooth, Highly Spherical Monocrystalline Gold Particles for Precision Plasmonics. ACS Nano. 2013;7 :11064–11070. Publisher's VersionAbstract
Ultrasmooth, highly spherical monocrystalline gold particles were prepared by a cyclic process of slow growth followed by slow chemical etching, which selectively removes edges and vertices. The etching process effectively makes the surface tension isotropic, so that spheres are favored under quasi-static conditions. It is scalable up to particle sizes of 200 nm or more. The resulting spherical crystals display uniform scattering spectra and consistent optical coupling at small separations, even showing Fano-like resonances in small clusters. The high monodispersity of the particles we demonstrate should facilitate the self-assembly of nanoparticle clusters with uniform optical resonances, which could in turn be used to fabricate optical metafluids. Narrow size distributions are required to control not only the spectral features but also the morphology and yield of clusters in certain assembly schemes.
2011
Fan JA, He Y, Bao K, Wu C, Bao J, Schade NB, Manoharan VN, Shvets G, Nordlander P, Liu DR, et al. DNA-Enabled Self-Assembly of Plasmonic Nanoclusters. Nano Letters. 2011;11 :4859–4864. Publisher's VersionAbstract
DNA nanotechnology provides a versatile foundation for the chemical assembly of nanostructures. Plasmonic nanoparticle assemblies are of particular interest because they can be tailored to exhibit a broad range of electromagnetic phenomena. In this Letter, we report the assembly of DNA-functionalized nanoparticles into heteropentamer clusters, which consist of a smaller gold sphere surrounded by a ring of four larger spheres. Magnetic and Fano-like resonances are observed in individual clusters. The DNA plays a dual role: it selectively assembles the clusters in solution and functions as an insulating spacer between the conductive nanoparticles. These particle assemblies can be generalized to a new class of DNA-enabled plasmonic heterostructures that comprise various active and passive materials and other forms of DNA scaffolding. DNA nanotechnology provides a versatile foundation for the chemical assembly of nanostructures. Plasmonic nanoparticle assemblies are of particular interest because they can be tailored to exhibit a broad range of electromagnetic phenomena. In this Letter, we report the assembly of DNA-functionalized nanoparticles into heteropentamer clusters, which consist of a smaller gold sphere surrounded by a ring of four larger spheres. Magnetic and Fano-like resonances are observed in individual clusters. The DNA plays a dual role: it selectively assembles the clusters in solution and functions as an insulating spacer between the conductive nanoparticles. These particle assemblies can be generalized to a new class of DNA-enabled plasmonic heterostructures that comprise various active and passive materials and other forms of DNA scaffolding.