Realizing efficient resonant coupling between spins of different energy scales has significant applications in spin-based quantum technologies, such as quantum sensing. We find that spins with disparate energies can exhibit efficient resonant coupling through the introduction of uneven energy modulation. In this study we apply our proposed method to a nitrogen-vacancy center in close proximity to nuclei. Computational simulations demonstrate that a specific dynamical switching of the electron-spin Rabi frequency enables efficient electron-nuclear coupling, yielding a substantially stronger quantum sensing signal and dynamic nuclear polarization compared to existing methods. This approach holds promise for applications in high-field nanoscale nuclear magnetic resonances as well as for low-power quantum control of nuclear spins.

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• Open quantum systems & decoherence
• Quantum control
• Quantum sensing