Efficient transfer of the quantum state of ensembles of electronic spins to nuclear spins is at the root of many novel quantum-based technologies. However, accomplishing this transfer requires magnetic fields aligned to specific crystalline axes or cryogenic temperatures, limiting the range of applications. Here, we observe fast Rabi oscillations on electron-nuclear spin exchanging transitions, coherent population trapping, and polarization of nuclear spin ensembles under ambient conditions and using uncritical magnetic field angles. For this, we employ nominally forbidden electron-nuclear spin transitions in ensembles of nitrogen-vacancy (NV) centers in diamond identically coupled to their own ${}^{14}\mathrm{N}$ nuclei. This technique is scalable and could thus push the sensitivity of NV sensors forward. It could also be applied to efficient long-lived storage of microwave photons and to the coupling of nuclear spins to mechanical oscillators in the resolved sideband regime.

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• Atomic spectra
• Coherent control
• Cooling & trapping
• Zeeman effect