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NV-diamonds have attracted keen interest for nanoscale sensing and spinmanipulation. In particular, the non-equilibrium electron spin polarizationafter optical excitation of single NV centers has successfully been transferredto nuclear spin baths in the surrounding of the defects. However, theseexperiments need to be extended to NV-ensembles which have promising practicalapplications in the hyperpolarization of bulk sample volumes for NMR signalenhancement. Here, we use a dense, shallow ensemble of NV-centers todemonstrate polarization transfer to nuclear spins in a well-defined compositediamond sample system. This allows us to address three different types ofnuclear spins in different positions with respect to the NV polarizationsource: from the close proximity of $^{13}$C inside the diamond lattice to theself-assembled molecular system consisting of $^{1}$H and $^{19}$F spinsoutside the diamond and over multiple interfaces. We show that ensemble NVexperiments face problems different from single NV experiments. In particular,using spinlock pulses, the inhomogeneously broadened ESR line of the NVensemble limits the minimal resonance linewidth with which the transferprotocol can occur. Furthermore, we compare the NV spin-polarization losses andpolarization transfer rates to the different nuclear baths and discuss the roleof spin-diffusion as detrimentally affecting the direct observation of nuclearpolarization build-up within the detection volume of nanoscale NV-NMRexperiments.

Polarization transfer from optically-pumped NV center ensembles to multinuclear spin baths