Attosecond control of electron dynamics in carbon monoxide

Laser pulses with stable electric field waveforms establish the opportunity to achieve coherent control on attosecond time scales. We present experimental and theoretical results on the steering of electronic motion in a multielectron system. A very high degree of light-waveform control over the directional emission of C⁺ and O⁺ fragments from the dissociative ionization of CO was observed. Ab initio based model calculations reveal contributions to the control related to the ionization and laser-induced population transfer between excited electronic states of CO⁺ during dissociation.