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arXiv:2610.17050

Optical Detection of Coherent Nuclear Spin Control in a Molecular System at Room Temperature

Eoin O. Irving, Ziqiu Huang, Max Attwood, Sam L. Bayliss, Sarah K. Mann

quant-phphysics.chem-phSubmitted Oct 12, 2026• Announced Oct 13, 2026
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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.

Comments
8 pages, 3 figures

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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^{14}14N nuclear spins in the photoexcited triplet state of the organic chromophore 6,13-diazapentacene. The strong hyperfine coupling between the electronic spin and 14^{14}14N 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.
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Optically addressable molecular triplet spins provide a chemically tunable platform for quantum application, but their coherence is often limited by interactions with surrounding spin baths. Here we demonstrate controlled suppression of nuclear-bath-induced decoherence in photoexcited triplet spins of pentacene co-crystallized in high-purity naphthalene single crystals. By hyperpolarizing the proton spin bath through triplet dynamic nuclear polarization (triplet-DNP), magnetic noise generated by the nuclear spins is suppressed, leading to an extension of the electron spin transverse coherence time. Experimentally, we observe a 25\% enhancement of the spin-echo decay time with 60%60\%60% polarization of the proton spin bath. The measured scaling of the spin-echo decay time (T2T_2T2​) with nuclear polarization quantitatively follows the predicted dependence derived from the polarization-controlled nuclear second moment. Both the enhancement and the absolute value of the coherence time are quantitatively reproduced by cluster correlation expansion (CCE) simulations. These results establish nuclear spin hyperpolarization as a general and actively tunable approach to engineering coherence in molecular qubits. This work provides a broadly applicable design framework for high-coherence molecular and solid-state spin systems.
Optically addressable shallow donors in ZnO combine efficient spin-selective optical transitions with the potential for long spin coherence in an isotopically purifiable host lattice, making them an attractive platform for spin-photon quantum technologies. A key missing capability, however, has been coherent control beyond the small-angle rotations accessible with ultrafast optical pulses. Here we demonstrate coherent microwave control of implanted 115In^{115}\mathrm{In}115In donors in ZnO. Resonant optical pumping initializes and reads out the donor electron spin. Pulsed optically-detected magnetic resonance resolves the ten hyperfine transitions associated with the coupled 115In^{115}\mathrm{In}115In nuclear spin (I = 9/2) and reveals optical-pumping-induced nuclear spin polarization. We observe coherent Rabi oscillations with a maximum Rabi frequency of Ω/2π=36.2±0.7Ω/2π= 36.2 \pm 0.7Ω/2π=36.2±0.7\;MHz, corresponding to a πππ-pulse time of 13.8$\pm$0.3\;ns, and characterize the spin coherence using Ramsey, Hahn echo and dynamical-decoupling measurements. Unexpectedly, the measured coherence is substantially shorter than reported in previous optical studies of donor spins in ZnO at high magnetic field. Control experiments rule out several simple explanations including microwave heating and instantaneous diffusion from the driven donor ensemble, leaving an open question regarding the origin of decoherence at low magnetic field in microwave-controlled ZnO donors. These results establish microwave control of ZnO donor qubits with resonant optical access to specific donor species. More broadly, they demonstrate that coherent microwave control can be achieved in optically addressable spin systems with nanosecond-scale inhomogeneous dephasing, enabling field-, temperature-, and materials-dependent studies of coherence-limiting mechanisms and the development of optically interfaced electron-nuclear spin registers.
Quantum sensors based on individual spins provide unprecedented access to local magnetic fields in condensed matter, chemistry, and biology, with solid-state defect spins emerging as the leading platform. However, their molecular-sensing capabilities are limited by confinement to a host lattice, which prevents placement in close proximity to a target molecule. Molecular spins offer an alternative, enabling chemical tunability and flexible positioning relative to the target system. Here we present a nanoscale sensing platform that combines molecular electron spins, ultrasensitive mechanical readout, and Hamiltonian engineering. Using a modified XYXY dipolar decoupling sequence, we suppress electron-electron dipolar interactions across a broad distribution of control fields, extending coherence times to ∼400 μ\sim 400~μ∼400 μs in an attoliter-scale droplet containing $\sim$100 trityl-OX063 radicals. Leveraging this sequence, we demonstrate frequency-selective detection of nanotesla-scale AC fields and perform sensing and spectroscopy of small, local nuclear-spin ensembles. Collectively, these results establish SQUINT (Spin-based QUantum Integrated Nanomechanical Transduction) as a framework for quantum sensing that affords molecular-level control over sensor properties and enables direct integration into complex molecular targets.
Nuclear spins in certain solids couple weakly to their environment, making them attractive candidates for quantum information processing and inertial sensing. When coupled to the spin of an optically active electron, nuclear spins can be rapidly polarized, controlled, and read via lasers and radio-frequency (rf) fields. Possessing typical coherence times of several milliseconds at room temperature, nuclear spins hosted by a nitrogen-vacancy center in diamond are thus intriguing systems to observe how classical physical rotation at quantum timescales affects a quantum system. In this work, we demonstrate optical nuclear-spin polarization and rapid quantum control of nuclear spins in a diamond physically rotating at 1kHz1\phantom{\rule{0.16em}{0ex}}\mathrm{kHz}1kHz, faster than the nuclear-spin coherence time. Free from the need to maintain strict field alignment, we are able to measure and control nuclear spins in the presence of a large, time-varying magnetic field that makes an angle of more than ${100}^{\ensuremath{\circ}}$ to the nitrogen-lattice vacancy axis. The field induces spin mixing between the electron and nuclear states of the qubits, decoupling them from oscillating rf fields. We are able to demonstrate that coherent spin state control is possible at any point of the rotation. We combine continuous dynamical decoupling with feed-forward control to eliminate decoherence induced by imperfect mechanical rotation. Our work liberates a previously inaccessible degree of freedom of the NV nuclear spin, unlocking new approaches to quantum control and rotation sensing.
Quantum sensing has witnessed rapid development and transition from laboratories to practical applications in the past decade. Applications of quantum sensors, ranging from nanotechnologies to biosensing, are expected to benefit from quantum sensors' unprecedented spatial resolution and sensitivity. Solid-state spin systems are particularly attractive platforms for quantum sensing technologies because room temperature operation is viable while reaching the quantum limits of sensitivity. Among various solid-state spin systems, nitrogen-vacancy (NV) centers in diamond demonstrated high-fidelity initialization, coherent control, and high contrast readout of the electron spin state. However, electron spin coherence due to noise from the surrounding spin bath and this environment effect limits the sensitivity of NV centers. Thus, a critical task in NV center-based quantum sensing is sensitivity enhancement through coherence protection. Several strategies, such as dynamical decoupling techniques, feedback control, and nuclear spin-assisted sensing protocols, have been developed and realized for this task. Among these strategies, nuclear spin-assisted protocols have demonstrated greater enhancement of electron spin coherence. In addition, the electron and nuclear spin pair of an NV center in diamond naturally allows the application of the nuclear spin-assisted sensitivity enhancement protocol. Owing to long nuclear coherence times, further enhancement of sensitivity can be achieved by exploiting active nuclear spins (e.g., 14N, 13C) in the proximity of an NV center as memory ancillas when coupled with the NV center. Here, we review the spin properties of NV centers, mechanisms of the nuclear spin-assisted protocol and its gate variation, and the status of quantum sensing applications in high-resolution nuclear spin spectroscopy, atomic imaging, and magnetic field sensing. We discuss the potential for commercialization, current challenges in sensitivity enhancement, and conclude with future research directions for promoting the development of nuclear spin-assisted protocol and its integration into industrial applications.