Double electron resonance with two ensembles of nitrogen-vacancy centers in diamond

Nitrogen-vacancy (NV) centers in diamond are widely used in the development of a number of sensors. The sensitivity of these devices is limited by both the number of centers used and their coherent properties. While the effects on the coherent properties of paramagnetic impurities such as carbon 13-isotopes and p1 centers are rather well understood, the mutual interaction of NV centers, which becomes especially important in relatively dense NV ensembles, is less well understood. Here, we provide a systematic study of NV-NV interaction using a dynamical double electron-electron resonance sequence, making it possible to directly observe the interaction of NV centers. Two types of dynamical DEER sequences were considered, consisting of 3 and 4 pulses. The nature of the phase jump in the 3-pulse sequence was attributed to the effect of non-commuting rotations within the sequence. Both the phase of the state vector rotation and its amplitude decay were studied, thus presenting a complete picture of decoherence due to NV-NV interaction. It was shown that the rate of the state vector decay differed significantly from predictions for a spin 1/2 system. However, the decay rate observed in the DEER sequence remained a reliable indicator of the concentration of bath spins and could be used to measure NV center concentration, provided that the magnetic transition of NV centers is saturated.