Dynamic Nuclear Polarization (DNP) has enabled enormous gains in magnetic
resonance signals and led to vastly accelerated NMR/MRI imaging and
spectroscopy. Unlike conventional cw-techniques, DNP methods that exploit the
full electron spectrum are appealing since they allow direct participation of
all electrons in the hyperpolarization process. Such methods typically entail
sweeps of microwave radiation over the broad electron linewidth to excite DNP,
but are often inefficient because the sweeps, constrained by adiabaticity
requirements, are slow. In this paper we develop a technique to overcome the
DNP bottlenecks set by the slow sweeps, employing a swept microwave frequency
comb that increases the effective number of polarization transfer events while
respecting adiabaticity constraints. This allows a multiplicative gain in DNP
enhancement, scaling with the number of comb frequencies and limited only by
the hyperfine-mediated electron linewidth. We demonstrate the technique for the
optical hyperpolarization of 13C nuclei in powdered microdiamonds at low
fields, increasing the DNP enhancement from 30 to 100 measured with respect to
the thermal signal at 7T. For low concentrations of broad linewidth electron
radicals, e.g. TEMPO, these multiplicative gains could exceed an order of
magnitude.Comment: Contains supplementary inf