Optically Detected Nuclear Magnetic Resonance Capsule: Data and Programs

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. In this capsule the data and programs are uploaded for the review process: - each plot in the manuscript was created with an python plot program, the corresponding data is uploaded in the data folders - Supplementary Information (SI) plots have their programs and folders - all plots created by the programs are saved in the results folder - more information can be found in the readme.txt documentation file