Controlling molecular isomerization and fragmentation with laser-induced electron recollision

In this submission, we present the first, to our knowledge, CEP control of fragmentation pathways of polyatomic molecules (acetylene, ethylene, 1,3-butadiene). Given the increased number of participating nuclei and a vastly more complex valence electron dynamics and the structure of energy surfaces, it is counterintuitive to expect the CEP dependence of fragmentation pathways to survive in polyatomic molecules. We argue both experimentally and theoretically, that such a universal attosecond mechanism of quasi-single-cycle fragmentation of large molecules is the field control of the tunneled-out electronic wave packet that is steered by the optical waveform before its recollision with the parent ion.