All-optical hyperpolarization of electron and nuclear spins in diamond

Low thermal polarization of nuclear spins is a primary sensitivity limitation for nuclear magnetic resonance. Here we demonstrate optically pumped (microwave-free) nuclear spin polarization of $¹³\mathrm{C}$ and $¹⁵\mathrm{N}$ in $¹⁵\mathrm{N}$-doped diamond. $¹⁵\mathrm{N}$ polarization enhancements up to $\ensuremath{-}2000$ above thermal equilibrium are observed in the paramagnetic system ${{\mathrm{N}}_{\mathrm{s}}}⁰$ . Nuclear spin polarization is shown to diffuse to bulk $¹³\mathrm{C}$ with NMR enhancements of $\ensuremath{-}200$ at room temperature and $\ensuremath{-}500$ at 240 K, enabling a route to microwave-free high-sensitivity NMR study of biological samples in ambient conditions.