Determining\nKey Factors for the Open-Loop Control\nof Molecular Fragmentation Using Shaped Strong Fields

Pulse shaping has\nlong been employed for tailoring femtosecond\nlaser pulses to study and control the fragmentation of polyatomic\nmolecules. In many cases, a physical explanation connecting the properties\nof the field to the observed control is difficult to ascertain. We\nutilized 80 bit binary spectral phase functions to parametrize and\nmap the search space, gaining insight into which pulse parameters\nmost impact the ion yield and fragmentation pattern for the relatively\nlarge triethylamine [N(C<sub>2</sub>H<sub>5</sub>)<sub>3</sub>] molecule.\nPulse structures used to control the <i>m</i>/<i>z</i> 86 branching ratio beyond a simple intensity dependence are identified\nand compared to pump–probe results. All of these findings are\nexplained in terms of control via a dissociative Rydberg state in\nthe neutral molecule. This methodology may be used to discover new\ncontrol mechanisms and shed light onto which pulse parameters most\ninfluence the interaction between strong field lasers and matter.