We utilize nonlinear absorption to design all-optical protocols that improve both charge state initialization and spin readout for the nitrogen-vacancy (NV) center in diamond. Non-monotonic variations in the equilibrium charge state as a function of visible and near-infrared (NIR) optical power are attributed to competing multiphoton absorption processes. In certain regimes, multicolor illumination enhances the steady-state population of the NVs negative charge state above 90%. At higher NIR intensities, selective ionization of the singlet manifold facilitates a protocol for spin-to-charge conversion that dramatically enhances the spin readout fidelity. We demonstrate a 6-fold increase in the signal-to-noise ratio for single-shot spin measurements and predict an orders-of-magnitude experimental speedup over traditional methods for emerging applications in magnetometry and quantum information science using NV spins.
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