  We studied the spin depolarization of ensembles of nitrogen-vacancy (NV)
centers in nitrogen-rich single crystal diamonds. We found a strong dependence
of the evolution of the polarized state in the dark on the concentration of NV
centers. At low excitation power, we observed a simple exponential decay
profile in the low-density regime and a paradoxical inverted exponential
profile in the high-density regime. At higher excitation power, we observed
complex behavior, with an initial sharp rise in luminescence signal after the
preparation pulse followed by a slower exponential decay. Magnetic field and
excitation laser power-dependent measurements suggest that the rapid initial
increase of the luminescence signal is related to recharging of the
nitrogen-vacancy centers (from neutral to negatively charged) in the dark. The
slow relaxing component corresponds to the longitudinal spin relaxation of the
NV ensemble. The shape of the decay profile reflects the interplay between two
mechanisms: the NV charge state conversion in the dark and the longitudinal
spin relaxation. These mechanisms, in turn, are influenced by ionization,
recharging and polarization dynamics during excitation. Interestingly, we found
that charge dynamics are dominant in NV-dense samples even at very feeble
excitation power. These observations may be important for the use of ensembles
of NV centers in precession magnetometry and sensing applications.
