Sensing the internal dynamics of individual nuclear spins or clusters of nuclear spins has recently become possible by observing the coherence decay of a nearby electronic spin: the weak magnetic noise is amplified by a periodic, multipulse decoupling sequence. However, it remains challenging to robustly infer underlying atomic-scale structure from decoherence traces in all but the simplest cases. We introduce Floquet spectroscopy as a versatile paradigm for analysis of these experiments and argue that it offers a number of general advantages. In particular, this technique generalizes to more complex situations, offering physical insight in regimes of many-body dynamics, strong coupling, and pulses of finite duration. As there is no requirement for resonant driving, the proposed spectroscopic approach permits physical interpretation of striking, but overlooked, coherence decay features in terms of the form of the avoided crossings of the underlying quasienergy eigenspectrum. This is exemplified by a set of “diamond-shaped” features arising for transverse-field scans in the case of single-spin sensing by nitrogen-vacancy centers in diamond. We also investigate applications for donors in silicon, showing that the resulting tunable interaction strengths offer highly promising future sensors.
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