Removing inhomogeneous broadening in cross-relaxation spectra via hole burning

Quantum relaxometry based on nitrogen-vacancy (NV) centers in diamond is an easy-to-use technique that detects magnetic noise by measuring the longitudinal relaxation of NV centers. It is favored in chemical and biological applications due to the robustness against imperfect spin control. By tuning the energy level, NV relaxometry can detect magnetic noise generated by other spins and obtain magnetic resonance spectra through cross relaxation. However, the inhomogeneous broadening of NV centers greatly limits the spectral resolution of cross-relaxation spectra. Here we demonstrate a hole-burning technique to remove the inhomogeneous broadening. We utilize a weak pump field to deplete specific NV centers during the relaxation measurement, which contribute a reverse signal in the cross-relaxation spectra with a much narrower linewidth. Our method retains the convenience and sensitivity of NV relaxometry, opening up new avenues for high-resolution magnetic resonance spectroscopy in complex scenarios.