We demonstrate quantum control of ^9Be^+ ions directly implemented by an optical frequency comb. Based on numerical simulations of the relevant processes in ^9Be^+ for different magnetic field regimes, we demonstrate a wide applicability when controlling the comb's spectral properties. We introduce a novel technique for the selective and efficient generation of a spectrally tailored narrow-bandwidth optical frequency comb near 313 nm. We experimentally demonstrate internal state control and

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... rnal-motional state coupling of ^9Be^+ ions implemented by stimulated-Raman manipulation using a spectrally optimized optical frequency comb. Our pulsed laser approach is a key enabling step for the implementation of quantum logic and quantum information experiments in Penning traps.