Deterministic and Scalable Quantum Light Generation in DNA Origami-Programmed Organic Molecule-MoS${}_2$ Monolayer Hybrids

Abstract

The functionalization of atomically-thin transition metal dichalcogenides (TMDs) with organic molecules is a promising approach for realizing nanoscale optoelectronic devices with tailored functionalities, such as quantum light generation or p-n junctions. However, achieving precise control over the molecules' positioning on the 2D material remains a significant challenge. Here, we overcome the limitations of solution- and vapor-deposition methods and use a DNA origami placement technique to spatially arrange thiol molecules on a chip surface at the single-molecule level with high assembly yields. We successfully integrated MoS${}_2$ monolayers with micron-scale thiol-origami patterns, achieving single-photon emission from thiol-induced localized excitons in MoS${}_2$. Our work lays a foundation for the chemical control of quantum emitters in atomically-thin semiconductors and enables the design and production of ultracompact 2D devices for quantum technologies.