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We demonstrate the optical initialization of a hole-spin qubit bound to anisoelectronic center (IC) formed by a pair of Te impurities in ZnSe, animpurity/host system providing high optical homogeneity, large electric dipolemoments, and long coherence times. The initialization scheme is based on thespin-preserving tunneling of a resonantly excited donor-bound exciton to apositively charged Te IC, thus forming a positive trion. The radiative decay ofthe trion within less than 50 ps leaves a heavy hole in a well-definedpolarization-controlled spin state. The initialization fidelity exceeds 98:5 %for an initialization time of less than 150 ps.

High-Fidelity and Ultrafast Initialization of a Hole Spin Bound to a Te Isoelectronic Center in ZnS