TY - JOUR A1 - Choi, Youngeun ED - Choi, Youngeun ED - Kotthoff, L. ED - Olejko, L. ED - Resch-Genger, Ute ED - Bald, Ilko T1 - DNA origami-based Förster resonance energy-transfer nanoarrays and their application as ratiometric sensors JF - ACS applied materials and interfaces N2 - DNA origami nanostructures provide a platform where dye molecules can be arranged with nanoscale accuracy allowing to assemble multiple fluorophores without dye−dye aggregation. Aiming to develop a bright and sensitive ratiometric sensor system, we systematically studied the optical properties of nanoarrays of dyes built on DNA Origami platforms using a DNA template that provides a high versatility of label choice at minimum cost. The dyes are arranged at distances, at which they efficiently interact by Förster resonance energy transfer (FRET). To optimize array brightness, the FRET efficiencies between the donor fluorescein (FAM) and the acceptor cyanine 3 were determined for different sizes of the array and for different arrangements of the dye molecules within the array. By utilizing nanoarrays providing optimum FRET efficiency and brightness, we subsequently designed a ratiometric pH nanosensor using coumarin 343 as a pH-inert FRET donor and FAM as a pHresponsive acceptor. Our results indicate that the sensitivity of a ratiometric sensor can be improved simply by arranging the dyes into a well-defined array. The dyes used here can be easily replaced by other analyte-responsive dyes, demonstrating the huge potential of DNA nanotechnology for light harvesting, signal enhancement, and sensing schemes in life sciences. KW - DNA KW - Nanoparticle KW - DNA Origami KW - Array KW - FRET KW - Dye KW - pH KW - Nanosensor KW - Fluorescence PY - 2018 DO - https://doi.org/10.1021/acsami.8b03585 SN - 1944-8244 SN - 1944-8252 VL - 10 IS - 27 SP - 23295 EP - 23302 PB - American Chemical Society CY - Washington, DC AN - OPUS4-45798 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER -