The decoherence and recoherence of charge migration in ionized 1-iodo-1,3-butadiyne

Charge migration in molecular ions arises from the complex interplay between electronic dynamics and nuclear motion, with decoherence and recoherence playing pivotal roles in spatiotemporal evolution of this process. In this work, we present a detailed theoretical study of charge migration in the ionized 1-iodo-1,3-butadiyne cation using ab initio quantum dynamics simulations. We analyze ultrafast charge migration along the molecular axis and quantify the nuclear wave packet overlap between the electronic ground and first excited states to elucidate the mechanisms underlying decoherence and recoherence. Our results reveal that only a few symmetry-preserving vibrational normal modes significantly influence the coherence dynamics. Furthermore, we show that nonadiabatic transitions and spin–orbit coupling have minimal impact on the core coherence evolution of charge migration in IC4H+.