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Optical illumination on negatively charged nitrogen-vacancy $(\mathrm{N}{\mathrm{V}}^{\ensuremath{-}})$ centers inevitably causes stochastic charge-state transitions between the $\mathrm{N}{\mathrm{V}}^{\ensuremath{-}}$ and the neutral charge state of the NV center. It limits the steady-state population of $\mathrm{N}{\mathrm{V}}^{\ensuremath{-}}$ to 5% at minimum (\ensuremath{\sim}610 nm) and 80% (\ensuremath{\sim}532 nm) at maximum in intrinsic diamond depending on the wavelength. Here, we show Fermi-level control by phosphorus doping generates 99.4 \ifmmode\pm\else\textpm\fi{} 0.1% $\mathrm{N}{\mathrm{V}}^{\ensuremath{-}}$ under 1-\ensuremath{\mu}W and 593-nm excitation which is close to maximum absorption of $\mathrm{N}{\mathrm{V}}^{\ensuremath{-}}$. The pure $\mathrm{N}{\mathrm{V}}^{\ensuremath{-}}$ shows a fivefold increase in luminescence and a fourfold enhancement of an optically detected magnetic resonance under 593-nm excitation compared with those in intrinsic diamond.

Pure negatively charged state of the NV center inn-type diamond