LASIM, Université de Lyon and CNRS UMR 5579, 43 Bd du 11 Novembre 1918, F69622 Villeurbanne Cedex, France.
J Chem Phys. 2012 Aug 7;137(5):054312. doi: 10.1063/1.4737926.
C(60) molecules highly excited in the nanosecond regime decay following ionization and dissociation by emitting a series of carbon dimers, as well as other small fragments if excitation is strong enough. The fragmentation mass spectrum and kinetic energy release of all charged fragments obtained in these experiments are interpreted within the framework of the Weisskopf theory, using a realistic Monte Carlo procedure in which the rates of all relevant decay channels are modeled using Arrhenius expressions. Comparison between the measurements and the simulated spectra allows the distribution of deposited energy to be accurately estimated. The dependence of the fragment kinetic energies on the laser fluence, found in the simulation but not observed in the experimental results, indicates that the small fragments are not necessarily emitted from small fullerenes resulting from C(60) by sequential decay. Rather, direct multifragmentation of C(60) is invoked to interpret the observed patterns. The possible role of post-ionization of neutral emitted fragments is discussed.
在纳秒级,高度激发的 C(60) 分子通过发射一系列碳二聚体以及其他小碎片来进行离解和离子化,从而实现衰减。在这些实验中获得的所有带电碎片的碎裂质谱和动能释放都在 Weisskopf 理论的框架内进行了解释,使用了一种现实的蒙特卡罗程序,其中使用 Arrhenius 表达式对所有相关的衰减通道的速率进行建模。将测量结果与模拟谱进行比较,可以准确估计沉积能量的分布。在模拟中发现但在实验结果中未观察到的碎片动能对激光强度的依赖性表明,这些小碎片不一定是从小的富勒烯中发射出来的,这些小富勒烯是通过 C(60) 的顺序衰减产生的。相反,直接的多碎裂被用来解释观察到的模式。还讨论了中性发射碎片的后电离的可能作用。