title: Distance dependence of single-fluorophore quenching by gold nanoparticles studied on DNA origami.
abstract: We study the distance-dependent quenching of fluorescence due to a metallic nanoparticle in proximity of a fluorophore. In our single-molecule measurements, we achieve excellent control over structure and stoichiometry by using self-assembled DNA structures (DNA origami) as a breadboard where both the fluorophore and the 10 nm metallic nanoparticle are positioned with nanometer precision. The single-molecule spectroscopy method employed here reports on the co-localization of particle and dye, while fluorescence lifetime imaging is used to directly obtain the correlation of intensity and fluorescence lifetime for varying particle to dye distances. Our data can be well explained by exact calculations that include dipole-dipole orientation and distances. Fitting with a more practical model for nanosurface energy transfer yields 10.4 nm as the characteristic distance of 50% energy transfer. The use of DNA nanotechnology together with minimal sample usage by attaching the particles to the DNA origami directly on the microscope coverslip paves the way for more complex experiments exploiting dye-nanoparticle interactions.
authors.affiliation: Physical and Theoretical Chemistry-NanoBioScience, TU Braunschweig, Hans-Sommer-Strasse 10, 38106 Braunschweig, Germany. g.acuna@tu-bs.de
authors.forename: Guillermo P
authors.initials: GP
authors.lastname: Acuna
authors.forename: Martina
authors.initials: M
authors.lastname: Bucher
authors.forename: Ingo H
authors.initials: IH
authors.lastname: Stein
authors.forename: Christian
authors.initials: C
authors.lastname: Steinhauer
authors.forename: Anton
authors.initials: A
authors.lastname: Kuzyk
authors.forename: Phil
authors.initials: P
authors.lastname: Holzmeister
authors.forename: Robert
authors.initials: R
authors.lastname: Schreiber
authors.forename: Alexander
authors.initials: A
authors.lastname: Moroz
authors.forename: Fernando D
authors.initials: FD
authors.lastname: Stefani
authors.forename: Tim
authors.initials: T
authors.lastname: Liedl
authors.forename: Friedrich C
authors.initials: FC
authors.lastname: Simmel
authors.forename: Philip
authors.initials: P
authors.lastname: Tinnefeld
mesh_terms: D004247:DNA / Q000737:chemistry*; D005456:Fluorescent Dyes / Q000737:chemistry*; D006046:Gold / Q000737:chemistry*; D053768:Metal Nanoparticles / Q000737:chemistry*; D036103:Nanotechnology / Q000379:methods*; D055095:Optics and Photonics; D013050:Spectrometry, Fluorescence
chemical_list: D005456:Fluorescent Dyes; D006046:Gold; D004247:DNA