Patterning programmable spin arrays on DNA origami for quantum technologies

Abstract: The controlled assembly of solid-state spins with nanoscale spatial precision is an outstanding challenge for quantum technology. Here, we combine DNA-based patterning with nitrogen-vacancy (NV) ensemble quantum sensors in diamond to form and sense programmable 2D arrays of spins. We use DNA origami to control the spacing of chelated Gd$^{3+}$ spins, as verified by the observed linear relationship between proximal NVs' relaxation rate, $1/T_1$, and the engineered number of Gd$^{3+}$ spins per origami unit. We further show that DNA origami provides a robust way of functionalizing the diamond surface with spins as it preserves the charge state and spin coherence of proximal, shallow NV centers. Our work enables the formation and interrogation of ordered, strongly interacting spin networks with applications in quantum sensing and quantum simulation. We quantitatively discuss the prospects of entanglement-enhanced metrology and high-throughput proteomics.