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We combine multi-channel electronic structure theory with quantum optimalcontrol to derive Raman pulse sequences that coherently populate a valenceexcited state. For a neon atom, Raman target populations of up to 13% areobtained. Superpositions of the ground and valence Raman states with acontrollable relative phase are found to be reachable with up to 4.5%population and phase control facilitated by the pump pulse carrier envelopephase. Our results open a route to creating core-hole excitations in moleculesand aggregates that locally address specific atoms and represent the first steptowards realization of multidimensional spectroscopy in the xuv and x-rayregimes.

Laser pulses for coherent xuv Raman excitation