Decoherence-assisted spectroscopy of a single Mg+ ion

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We describe a high-resolution spectroscopy method, in which the detection of single excitation events is enhanced by a complete loss of coherence of a superposition of two ground states. Thereby, transitions of a single isolated atom nearly at rest are recorded efficiently with high signal-to-noise ratios. Spectra display symmetric line shapes without stray-light background from spectroscopy probes. We employ this method on a ²⁵Mg+ ion to measure one, two, and three-photon transition frequencies from the 3S ground state to the 3P, 3D, and 4P excited states, respectively. Our results are relevant for astrophysics and searches for drifts of fundamental constants. Furthermore, the method can be extended to other transitions, isotopes, and species. The currently achieved fractional frequency uncertainty of 5 × 10⁻⁹ is not limited by the method.