Phase control of molecular fragmentation with a pair of femtosecond-laser pulses

We demonstrate the control of molecular fragmentation of o-xylene (C(8)H(10)) on a femtosecond time scale in two-pulse measurements with a pair of femtosecond-laser pulses. Parent and fragment-ion yields were recorded as a function of interpulse delays, i.e., different relative phases of the excitation pulses. The experiments revealed different fragmentation mechanisms in the temporal region of direct overlapping pulses and for separated pulses. For overlapping pulses all ion yields followed the excitation intensity which oscillated as a function of interpulse delay due to the change of constructive and destructive interference of the light fields. For larger delays, in particular, the oscillations of the C(+) and CH(3) (+) fragment-ion yield showed a significant deviation from each other. The results are interpreted as a manifestation of optical phase-dependent electronic excitations mapped onto the nuclear fragmentation dynamics.