Quantum nonlinear spectroscopy of single nuclear spins

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Abstract

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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Meinel, J., Vorobyov, V., Wang, P., Yavkin, B., Pfender, M., Sumiya, H., … Wrachtrup, J. (2022). Quantum nonlinear spectroscopy of single nuclear spins. Nature Communications, 13(1). https://doi.org/10.1038/s41467-022-32610-8

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