Quantum nonlinear spectroscopy of single nuclear spins

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. Signals that look the same from their low-order correlations can often be distinguished by looking at higher-order ones. Here, the authors exploit the sensitivity of quantum nonlinear spectroscopy to fourth-order correlations to identify Gaussian noises, random-phased AC fields, and quantum spins.

Automated summary

Conventional nonlinear spectroscopy can only access a limited set of correlations in a quantum system, while quantum nonlinear spectroscopy can extract arbitrary types and orders of correlations. The authors used quantum nonlinear spectroscopy to measure fourth-order correlations and identified Gaussian noises, random-phased AC fields, and quantum spins.