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Resonance-inclined optical nuclear spin polarization of liquids in diamond structures

Dynamic nuclear polarization (DNP) of molecules in a solution at room temperature has potential to revolutionize nuclear magnetic resonance spectroscopy and imaging. The prevalent methods for achieving DNP in solutions are typically most effective in the regime of small interaction correlation times between the electron and nuclear spins, limiting the size of accessible molecules. To solve this limitation, we design a mechanism for DNP in the liquid phase that is applicable for large interaction correlation times. Importantly, while this mechanism makes use of a resonance condition similar to solid-state DNP, the polarization transfer is robust to a relatively large detuning from the resonance due to molecular motion. We combine this scheme with optically polarized nitrogen vacancy (NV) center spins in nanodiamonds to design a setup that employs optical pumping and is therefore not limited by room temperature electron thermal polarisation. We illustrate numerically the effectiveness of the model in a flow cell containing nanodiamonds immobilized in a hydrogel, polarising flowing water molecules 4700-fold above thermal polarisation in a magnetic field of 0.35 T, in volumes detectable by current NMR scanners.