The electronic spins of the nitrogen-vacancy (NV) centers in chemical-vapor-deposition (CVD) grown diamonds form ideal probes of magnetic fields and temperature, as well as promising qubits for quantum information processing. Studying and controlling the magnetic environment of NV centers in such high-purity crystals is thus essential for these applications. We demonstrate optical detection of paramagnetic species, such as hydrogen-related complexes, in a CVD-grown diamond. The resonant transfer of the NV centers' polarized electronic spins to the electronic spins of these species generates conspicuous features in the NV photoluminescence when employing magnetic field scans along the [100] crystal direction. Our results offer prospects for more detailed studies of CVD-grown processes as well as for coherent control of the spin of novel classes of hyperpolarized paramagnetic species.

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• Electronic structure of atoms & molecules
• Fine & hyperfine structure
• Nitrogen vacancy centers in diamond