title: High precision and high yield fabrication of dense nanoparticle arrays onto DNA origami at statistically independent binding sites.
abstract: High precision, high yield, and high density self-assembly of nanoparticles into arrays is essential for nanophotonics. Spatial deviations as small as a few nanometers can alter the properties of near-field coupled optical nanostructures. Several studies have reported assemblies of few nanoparticle structures with controlled spacing using DNA nanostructures with variable yield. Here, we report multi-tether design strategies and attachment yields for homo- and hetero-nanoparticle arrays templated by DNA origami nanotubes. Nanoparticle attachment yield via DNA hybridization is comparable with streptavidin-biotin binding. Independent of the number of binding sites, >97% site-occupation was achieved with four tethers and 99.2% site-occupation is theoretically possible with five tethers. The interparticle distance was within 2 nm of all design specifications and the nanoparticle spatial deviations decreased with interparticle spacing. Modified geometric, binomial, and trinomial distributions indicate that site-bridging, steric hindrance, and electrostatic repulsion were not dominant barriers to self-assembly and both tethers and binding sites were statistically independent at high particle densities.
authors.affiliation: Department of Materials Science & Engineering, Boise, ID 83725, USA. WillHughes@boisestate.edu.
authors.forename: Sadao
authors.initials: S
authors.lastname: Takabayashi
authors.forename: William P
authors.initials: WP
authors.lastname: Klein
authors.forename: Craig
authors.initials: C
authors.lastname: Onodera
authors.forename: Blake
authors.initials: B
authors.lastname: Rapp
authors.forename: Juan
authors.initials: J
authors.lastname: Flores-Estrada
authors.forename: Elias
authors.initials: E
authors.lastname: Lindau
authors.forename: Lejmarc
authors.initials: L
authors.lastname: Snowball
authors.forename: Joseph T
authors.initials: JT
authors.lastname: Sam
authors.forename: Jennifer E
authors.initials: JE
authors.lastname: Padilla
authors.forename: Jeunghoon
authors.initials: J
authors.lastname: Lee
authors.forename: William B
authors.initials: WB
authors.lastname: Knowlton
authors.forename: Elton
authors.initials: E
authors.lastname: Graugnard
authors.forename: Bernard
authors.initials: B
authors.lastname: Yurke
authors.forename: Wan
authors.initials: W
authors.lastname: Kuang
authors.forename: William L
authors.initials: WL
authors.lastname: Hughes
mesh_terms: D001665:Binding Sites; D004247:DNA / Q000737:chemistry* / Q000378:metabolism; D006046:Gold / Q000737:chemistry; D053768:Metal Nanoparticles / Q000737:chemistry*; D046228:Microarray Analysis / Q000295:instrumentation* / Q000706:statistics & numerical data; D018625:Microscopy, Atomic Force; D055616:Microtechnology / Q000379:methods; D036103:Nanotechnology / Q000379:methods; D043942:Nanotubes / Q000737:chemistry*; D009690:Nucleic Acid Conformation; D010316:Particle Size; D011336:Probability; D055672:Static Electricity; D013499:Surface Properties
chemical_list: D006046:Gold; D004247:DNA