Pumping of Nuclear Spins by Optical Excitation of Spin-Forbidden Transitions in a Quantum Dot

We demonstrate that efficient optical pumping of nuclear spins in semiconductor quantum dots (QDs) can be achieved by resonant pumping of optically forbidden transitions. This process corresponds to oneto-one conversion of a photon absorbed by the dot into a polarized nuclear spin, and also has potential for initialization of hole spin in QDs. We find that by employing this spin-forbidden process, nuclear polarization of 65% can be achieved, markedly higher than from pumping the allowed transition, which saturates due to the low probability of electron-nuclear spin flip-flop.