Charge-transfer as a mechanism for controlling molecular fragmentation

We investigate control over molecular fragmentation in the halogen substituted acetone 1,1-dibromo-3,3,3-trifluoroacetone using shaped ultrafast laser pulses. Following insight gained from closed-loop learning control experiments, further tests reveal that control over the CF3+/CHBr2+ ratio exploits a charge-transfer mechanism. We interpret the control in terms of adiabatic rapid passage.