Optically addressable spins, traditionally studied in semiconductors and, more recently, in (bio)chemical systems, are central to quantum technologies, yet existing platforms lack scalable and accessible site-specific programmability. Here, we show that DNA can serve as a functional nanoscale scaffold for optically addressable spin systems. By incorporating flavin chromophores into synthetic oligonucleotides, we generate spin-correlated radical pairs (SCRPs) that can be manipulated by radiofrequency (RF) fields and read out using optically detected magnetic resonance (ODMR). Pulsed ODMR resolves spin dynamics on sub-microsecond timescales under ambient conditions, while DNA sequence design enables atomically precise tuning of both the ODMR response and the associated spin chemistry with single-base resolution. DNA secondary structure provides an additional layer of functionality: duplex formation inverts the pulsed ODMR contrast, indicating a switch in the spin multiplicity of the SCRP precursor. The synthetic accessibility and chemical programmability of oligo-nucleotides as hosts for optically addressable spins are demonstrated through a series of proof-of-concept applications, including sensing, programmable SCRP positioning, and spin-enhanced molecular beacons. Our results establish DNA as a versatile scaffold for engineered spin systems, providing a platform for future applications ranging from quantum sensing and programmable spin arrays to bioimaging and RF-controlled molecular switches for gene regulation.
Meng, K., Einholz, C., Krueger, L., Rosenow, M., Bucher, D.
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