Optically detected nuclear magnetic resonance of coherent spins in a molecular complex

2025/09/01 by Evgenij Vasilenko, Vasilenko, Evgenij, Vishnu Unni Chorakkunnath +15
Physics and Astronomy · Chemistry · Materials Science · #Quantum optics and atomic interactions #Advanced NMR Techniques and Applications #Lanthanide and Transition Metal Complexes

paper · pdf · doi:10.48550/arxiv.2509.01467

Abstract

Nuclear magnetic resonance (NMR) is a powerful tool for applications ranging from chemical analysis to quantum information processing. Achieving optical initialization and detection of molecular nuclear spins promises new opportunities - including improved NMR signals at low magnetic field, sensitivity down to the single-molecule level, and full access to atomically precise molecular architectures for quantum technologies. In this study, we report optical readout of coherently controlled nuclear spins in a europium-based molecular crystal. By harnessing ultra-narrow optical transitions, we achieve optical initialization and detection of nuclear spin states. Through radio-frequency driving, we address two nuclear quadrupole resonances, characterized by narrow inhomogeneous linewidths and a distinct correlation with the optical transition frequency. We implement Rabi oscillations, spin echo and dynamical decoupling techniques, achieving nuclear spin quantum coherence with a lifetime of up to 2 ms. These results highlight the capabilities of optically detected NMR (ODNMR) and underscore the potential of molecular nuclear spins for quantum information processing.

Citations

• A high-resolution molecular spin-photon interface at telecommunications wavelengths
• Minute-long quantum coherence enabled by electrical depletion of magnetic noise
• Nuclear Spin Engineering for Quantum Information Science
• High sensitivity pressure and temperature quantum sensing in organic crystals
• Optical read and write of spin states in organic diradicals
• High fidelity optical readout of a nuclear spin qubit in Silicon Carbide
• Optical coherence and spin population dynamics in ¹⁷¹Yb³⁺:Y₂SiO₅ single crystals
• Guiding Diamond Spin Qubit Growth with Computational Methods
• Enhancing Spin Coherence in Optically Addressable Molecular Qubits through Host-Matrix Control
• Robust quantum-network memory based on spin qubits in isotopically engineered diamond

Cited by

• Bipartite entanglement in a nuclear spin register mediated by a quasi-free electron spin

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• Nuclear magnetic resonance on a single atom with a local probe
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• Molecule-based coherent light-spin interfaces for quantum information processing -- optical spin state polarization in a binuclear Europium complex