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The paper demonstrates optically detected Rabi oscillations of ¹⁴N nuclear spins in a photoexcited molecular triplet state at room temperature, which is a concrete step toward using molecular nuclear spins as quantum memories. The result is an early proof of coherent control, not a deployed sensor, and the sensing gains it targets remain prospective. For quantum readers, the key points are that room-temperature operation removes a major cryogenic barrier and that hyperfine coupling to the electron spin speeds up nuclear rotations.
Optical Detection of Coherent Nuclear Spin Control in a Molecular System at Room Temperature
arXiv:2610.17050v1 Announce Type: new Abstract: Molecular systems with optically addressable electron spins are emerging as versatile quantum sensing platforms, offering tunable qubit properties and molecular-scale spatial control. Owing to their longer lifetimes, coupled nuclear spins provide an attractive resource for enhancing sensing performance. For molecular spin systems, the ability to initialise, coherently control and readout nuclear spins at room temperature is crucial for realising such benefits. Here, we present the first optical detection of nuclear magnetic resonance and coherent nuclear spin control with a molecular system at room temperature. Specifically, we demonstrate optically detected Rabi oscillations of $^{14}$N nuclear spins in the photoexcited triplet state of the organic chromophore 6,13-diazapentacene. The strong hyperfine coupling between the electronic spin and $^{14}$N nuclei enhances the nuclear Rabi frequency, enabling fast coherent nuclear-spin rotations. This work lays the foundation for leveraging nuclear spins as memories for enhanced molecular-based quantum sensing.
Abstract:Molecular systems with optically addressable electron spins are emerging as versatile quantum sensing platforms, offering tunable qubit properties and molecular-scale spatial control. Owing to their longer lifetimes, coupled nuclear spins provide an attractive resource for enhancing sensing performance. For molecular spin systems, the ability to initialise, coherently control and readout nuclear spins at room temperature is crucial for realising such benefits. Here, we present the first optical detection of nuclear magnetic resonance and coherent nuclear spin control with a molecular system at room temperature. Specifically, we demonstrate optically detected Rabi oscillations of $^{14}$N nuclear spins in the photoexcited triplet state of the organic chromophore 6,13-diazapentacene. The strong hyperfine coupling between the electronic spin and $^{14}$N nuclei enhances the nuclear Rabi frequency, enabling fast coherent nuclear-spin rotations. This work lays the foundation for leveraging nuclear spins as memories for enhanced molecular-based quantum sensing.
Quantum Physics (quant-ph); Chemical Physics (physics.chem-ph)
arXiv:2610.17050 [quant-ph]
(or arXiv:2610.17050v1 [quant-ph] for this version)
https://doi.org/10.48550/arXiv.2610.17050 Focus to learn more arXiv-issued DOI via DataCite (pending registration)
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