DNA self-assembly of single molecules with deterministic position and orientation

TL;DR

This paper demonstrates a method to precisely control the orientation of single molecules on DNA origami structures, enabling advanced nanodevice fabrication with specific molecular alignments.

Contribution

It introduces a novel approach to orient individual molecules using unpaired bases in DNA origami, achieving controlled perpendicular and parallel orientations.

Findings

Achieved controlled molecular orientation with 0 and 8 unpaired bases.

Demonstrated potential applications in energy transfer and nano-antennas.

Expanded DNA origami capabilities for nanodevice engineering.

Abstract

An ideal nanofabrication method should allow the organization of nanoparticles and molecules with nanometric positional precision, stoichiometric control and well-defined orientation. The DNA origami technique has evolved into a highly versatile bottom-up nanofabrication methodology that fulfils almost all of these features. It enables the nanometric positioning of molecules and nanoparticles with stoichiometric control, and even the orientation of asymmetrical nanoparticles along predefined directions. However, orienting individual molecules has been a standing challenge, mainly due to unspecific electrostatic interactions. Here, we show how single molecules, namely Cy5 and Cy3 fluorophores, can be incorporated in a DNA origami with controlled orientation by doubly linking them to oligonucleotide strands that are hybridized while leaving enough unpaired bases to induce a stretching force. Particularly, we explore the effects of leaving 0, 2, 4, 6, and 8 unpaired bases and find extreme orientations for 0 and 8 unpaired bases, corresponding to the molecules being perpendicular and parallel to the DNA double helix, respectively. We foresee that these results will expand the application field of DNA origami towards the fabrication of nanodevices involving a wide range of orientation-dependent molecular interactions, such as energy transfer, intermolecular electron transport, catalysis, exciton delocalization, or the electromagnetic coupling of a molecule to specific resonant nano-antennas modes.