Based on both, ab-initio cluster calculations as well as periodic density functional based loss function calculations, we have assigned the origins of the valence electron excitation regime in electron energy loss spectra of well-ordered ceria films in (111) orientation at various states of reduction as well as after exposing the reduced films to hydrogen from the gas phase (Li et al, Angew. Chem. Int. Ed., 58 (2019) 14686–14693). The explicit calculation of intensity distributions using the dipole approximation allow us to draw conclusions about the nature of oxygen vacancies, which occur upon reduction and how those interact with hydrogen to form hydride species.

The present study also reports a brief discussion of vibrational excitations of hydrogen loaded ceria and corroborates previous interpretations, based on inelastic neutron scattering.

基于从头算簇计算以及基于周期性密度泛函的损失函数计算，我们在各种状态下以（111）取向的有序二氧化铈薄膜的电子能量损失谱中分配了价电子激发状态的起源还原以及将还原膜暴露于气相中的氢气后（Li et al, Angew. Chem. Int. Ed., 58 (2019) 14686-14693）。使用偶极近似对强度分布的明确计算使我们能够得出关于在还原时发生的氧空位的性质以及它们如何与氢相互作用形成氢化物物种的结论。

本研究还简要讨论了载氢二氧化铈的振动激发，并证实了基于非弹性中子散射的先前解释。