We present a combined experimental and theoretical study of the fragmentation of molecular CS₂ after sulfur 1s Auger cascade decay, consisting of electron–multi-ion coincidence spectra of charged fragments and theoretical simulations combining density functional theory and molecular dynamics. On the experimental side, a procedure for a complete determination of all sets of ions formed is described. For many of the fragmentation channels, we observed a higher charge in one of the sulfur atoms than the other atoms. Based on these observations and the theoretical simulations where the time scale of the nuclear motion and decay is taken into account, we propose that KLL Auger decay after the 1s core hole creation, via 2p double hole states, results in highly charged and strongly repulsive states with one localized core hole. These localized core holes are sufficiently long-lived that some will decay after fragmentation of the molecular ion, thereby efficiently impeding charge exchange between the fragments.

我们提出了结合的实验和理论研究的分子CS ₂的碎片硫1s俄歇级联衰变后，由带电碎片的电子-多离子重合谱以及结合密度泛函理论和分子动力学的理论模拟组成。在实验方面，描述了用于完全确定形成的所有离子集的过程。对于许多碎片通道，我们观察到一个硫原子比另一个原子具有更高的电荷。根据这些观察结果和考虑到核运动和衰变的时间尺度的理论模拟，我们建议在1s核心孔产生之后，通过2p双孔态产生的KLL Auger衰变会导致高度带电和强烈排斥状态有一个局部的芯孔。这些局部的核心孔具有足够长的寿命，以至于某些分子离子碎裂后会衰减，