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This study explores the strong-field dissociative ionization dynamics of $\mathrm{CF_2I_2}$ by manipulating initial rotational-state distributions using an electrostatic deflector. The results reveal that even minor adjustments in rotational energy can significantly influence ion-channel branching ratios and fragmentation dynamics, highlighting the critical role of rotational excitation. The findings indicate that non-adiabatic Coriolis-type coupling plays a pivotal role in determining the competition between stabilization into bound ionic states and dissociative channels.
Minor tweaks in rotational energy can drastically alter ionization dynamics and product distributions in $\mathrm{CF_2I_2}$, revealing a new layer of control in molecular fragmentation processes.
We investigated strong-field dissociative ionization of $\mathrm{CF_2I_2}$ ensembles prepared in different initial rotational-state distributions using an electrostatic deflector. Pronounced changes in ion-channel branching ratios revealed a strong dependence of the fragmentation dynamics on the initial rotational excitation. Analysis of fragment yields and their laser-power dependences identifies resonance-enhanced multiphoton ionization through an intermediate excited state, $\mathrm{CF_2I_2^{\ast}}$. The measured branching behavior indicates competition between stabilization into bound ionic states and dissociative channels, driven by near-threshold non-adiabatic Coriolis-type coupling. Tuning the rotational energy by only a few $\mu$eV is sufficient to significantly alter the ionization dynamics and to redistribute the reaction products. These findings demonstrate the key role of rotational excitation in controlling non-adiabatic dynamics following strong-field ionization of $\mathrm{CF_2I_2}$.
