Abstract
Magnetic noise of atomic nuclear spins is a major problem for solid state spin qubits. Highly-polarized nuclei would not only overcome this obstacle, but also make nuclear spins a useful quantum information resource. However, achieving sufficiently high nuclear polarizations has remained an evasive goal. Here we implement a nuclear spin polarization protocol which combines strong optical pumping and fast electron tunneling. Polarizations well above 95% are generated in GaAs semiconductor quantum dots on a timescale of 1 minute. The technique is compatible with standard quantum dot device designs, where highly-polarized nuclear spins can simplify implementations of quantum bits and memories, as well as offer a testbed for studies of many-body quantum dynamics and magnetism.