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    Quantum nonlinear spectroscopy of single nuclear spins
    (2022) Meinel, Jonas; Vorobyov, Vadim; Wang, Ping; Yavkin, Boris; Pfender, Mathias; Sumiya, Hitoshi; Onoda, Shinobu; Isoya, Junichi; Liu, Ren-Bao; Wrachtrup, Jörg
    Conventional nonlinear spectroscopy, which use classical probes, can only access a limited set of correlations in a quantum system. Here we demonstrate that quantum nonlinear spectroscopy, in which a quantum sensor and a quantum object are first entangled and the sensor is measured along a chosen basis, can extract arbitrary types and orders of correlations in a quantum system. We measured fourth-order correlations of single nuclear spins that cannot be measured in conventional nonlinear spectroscopy, using sequential weak measurement via a nitrogen-vacancy center in diamond. The quantum nonlinear spectroscopy provides fingerprint features to identify different types of objects, such as Gaussian noises, random-phased AC fields, and quantum spins, which would be indistinguishable in second-order correlations. This work constitutes an initial step toward the application of higher-order correlations to quantum sensing, to examining the quantum foundation (by, e.g., higher-order Leggett-Garg inequality), and to studying quantum many-body physics.
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    Photo-induced ionization dynamics of the nitrogen vacancy defect in diamond investigated by single-shot charge state detection
    (2013) Aslam, Nabeel; Waldherr, Gerald; Neumann, Philipp; Jelezko, Fedor; Wrachtrup, Jörg
    The nitrogen-vacancy centre (NV) has drawn much attention for over a decade, yet detailed knowledge of the photophysics needs to be established. Under typical conditions, the NV can have two stable charge states, negative (NV-) or neutral (NV0), with photo-induced interconversion of these two states. Here, we present detailed studies of the ionization dynamics of single NV centres in bulk diamond at room temperature during illumination and its dependence on the excitation wavelength and power. We apply a recent method which allows us to directly measure the charge state of a single NV centre, and observe its temporal evolution. We find that the steady-state NV− population is always ⩽75% for 450–610 nm excitation wavelength. In combination with saturation measurements, we show that the optimal excitation wavelength is around 510-540 nm. Furthermore, the relative absorption cross-section of NV- is determined for 540-610 nm, revealing a double-peak structure. Finally, the energy of the NV- ground state of 2.6 eV below the conduction band is measured. These results reveal new insights into the charge state dynamics of the NV centre.