  We investigate spin-dependent decay and intersystem crossing in the optical
cycle of single negatively-charged nitrogen-vacancy (NV) centres in diamond. We
use spin control and pulsed optical excitation to extract both the
spin-resolved lifetimes of the excited states and the degree of
optically-induced spin polarization. By optically exciting the centre with a
series of picosecond pulses, we determine the spin-flip probabilities per
optical cycle, as well as the spin-dependent probability for intersystem
crossing. This information, together with the indepedently measured decay rate
of singlet population provides a full description of spin dynamics in the
optical cycle of NV centres. The temperature dependence of the singlet
population decay rate provides information on the number of singlet states
involved in the optical cycle.
