Efficient hyperpolarization of nuclear spins via optically active defect centers, such as the nitrogen vacancy (NV) center in diamond, has great potential for enhancing NMR-based quantum information processing and nanoscale magnetic resonance imaging. Recently, pulse-based protocols have been shown to efficiently transfer optically induced polarization of the electron defect spin to surrounding nuclear spins - at particular resonant pulse intervals. In this work, we investigate the performance of these protocols, both analytically and experimentally, with the electronic spin of a single NV defect. We find that whenever polarization resonances of nuclear spins are near degenerate with a "blocking"spin, which is single spin with stronger off-diagonal coupling to the electronic central spin, they are displaced out of the central resonant region - without, in general, significant weakening in the rate of polarization. We analyze the underlying physical mechanism and obtain a closed-form expression for the displacement. We propose that spin blocking represents a common but overlooked effect in hyperpolarization of nuclear spins and suggest solutions for improved protocol performance in the presence of (naturally occurring) blocking nuclear spins.

The use of the nuclear spins surrounding electron spin qubits as quantum registers and long-lived memories opens the way to new applications in quantum information and biological sensing. Hence, there is a need for generic and robust forms of control of the nuclear registers. Although adiabatic gates are widely used in quantum information, they can become too slow to outpace decoherence. Here, we introduce a technique whereby adiabatic gates arise from the dynamical decoupling protocols that simultaneously extend coherence. We illustrate this pulse-based adiabatic control for nuclear spins around NV centers in diamond. We obtain a closed-form expression from Landau-Zener theory and show that it reliably describes the dynamics. By identifying robust Floquet states, we show that the technique enables polarization, one-shot flips, and state storage for nuclear spins. These results introduce a control paradigm that combines dynamical decoupling with adiabatic evolution.