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An ultimate goal of electron paramagnetic resonance (EPR) spectroscopy is toanalyze molecular dynamics in place where it occurs, such as in a living cell.The nanodiamond (ND) hosting nitrogen-vacancy (NV) centers will be a promisingEPR sensor to achieve this goal. However, ND-based EPR spectroscopy remainselusive, due to the challenge of controlling NV centers without well-definedorientations inside a flexible ND. Here, we show a generalized zero-field EPRtechnique with spectra robust to the sensor's orientation. The key is applyingan amplitude modulation on the control field, which generates a series ofequidistant Floquet states with energy splitting being theorientation-independent modulation frequency. We acquire the zero-field EPRspectrum of vanadyl ions in aqueous glycerol solution with embedded single NDs,paving the way towards \emph{in vivo} EPR.

In situ electron paramagnetic resonance spectroscopy using single nanodiamond sensors