High-resolution and wide-frequency-range magnetic spectroscopy with solid-state spin ensembles

Quantum systems composed of solid-state electronic spins can be sensitive detectors of narrowband magnetic fields. A prominent example is the nitrogen-vacancy (NV) center in diamond, which has been employed for magnetic spectroscopy with high spatial and spectral resolution. However, NV-diamond spectroscopy protocols are typically based on dynamical decoupling sequences, which are limited to low-frequency signals ( ≲ 20 MHz) due to the technical requirements on microwave (MW) pulses used to manipulate NV electronic spins. In this work, we experimentally demonstrate a high-resolution magnetic spectroscopy protocol that integrates a quantum frequency mixing (QFM) effect in a dense NV ensemble with coherently averaged synchronized readout (CASR) to provide both a wide range of signal frequency detection and sub-Hz spectral resolution. We assess the sensitivity of this QFM-CASR protocol across a frequency range of 10 MHz to 4 GHz. By measuring the spectra of multi-frequency signals near 0.6, 2.4 and 4 GHz, we demonstrate sub-Hz spectral resolution with a nT-scale noise floor for the target signal, and precise phase measurement with error < 1∘. Compared to state-of-the-art NV-diamond techniques for high-resolution magnetic spectroscopy, the QFM-CASR protocol extends the signal frequency range by more than an order of magnitude, enabling applications in radio frequency (RF) and MW signal microscopy and analysis, as well as tesla-scale nuclear magnetic resonance (NMR) spectroscopy of small samples.