Cavity-assisted dynamic nuclear polarisation

Dynamic nuclear polarisation transfers polarisation from electron to nuclear spins by relying on a dissipative channel. Here we introduce a cavity-based DNP mechanism which uses the radiative relaxation of the electronic spin through the Purcell effect to bring about the nuclear spin polarisation. We implement this protocol on an ensemble of bismuth donor spins (I=9/2, S=1/2) in isotopically purified silicon coupled to a superconducting resonator. A single cycle, combining adiabatic microwave and radio-frequency pulses with Purcell relaxation, increases a target ground state's population by a factor of 1.79 plus or minus0.04; a cumulative enhancement of 4.6 plus or minus0.2 is reached with additional cycles, to be compared with the theoretical limit of ninefold set by the degeneracy of the ground manifold. We explain this difference by the competition between Purcell and intrinsic relaxation on the one hand and a collective effect that slows down the electronic spin radiative decay as the nuclear spin population grows on the other hand. Our results place radiative DNP as an available mechanism at millikelvin temperatures where phonon-mediated relaxation is frozen.