第一排过渡金属氧化物XUV基态和激发态的从头计算
Ab Initio Calculations of XUV Ground and Excited States for First-Row Transition Metal Oxides
摘要：
瞬态X射线光谱学由于其对载流子占据和局部化学或结构动力学的敏感性而在研究太阳能材料中的光激发动力学中变得无处不在。然而，固态光激发动力学的解释是复杂的核心孔扰动和由此产生的多体动力学。在这里，从头算，贝特-萨尔彼得方程（BSE）的方法开发，可以将固态材料的光激发态效应。第一行过渡金属氧化物- $TiO_2, α-Cr_2O_3, β-MnO_2, α-Fe_2O_3, Co_3O_4, NiO, CuO, and ZnO$ -的基态，光激发态和热膨胀态的极紫外（XUV）吸收光谱的计算证明这种方法的准确性。该理论被用来分解的核心价态激子的X射线跃迁哈密顿量为每个过渡金属氧化物的调查到单独的组件。分解提供了一个物理直观的XUV光谱特征的起源，以及光谱将如何改变以下光激发。该方法很容易推广到其他K，L，M和N的边缘提供了一个通用的方法来分析瞬态X射线吸收或反射数据。
英文摘要：
Transient X-ray spectroscopies have become ubiquitous in studying photoexcited dynamics in solar energy materials due to their sensitivity to carrier occupations and local chemical or structural dynamics. The interpretation of solid-state photoexcited dynamics, however, is complicated by the core-hole perturbation and the resulting many-body dynamics. Here, an ab initio, Bethe-Salpeter equation (BSE) approach is developed that can incorporate photoexcited state effects for solid-state materials. The extreme ultraviolet (XUV) absorption spectra for the ground, photoexcited, and thermally expanded states of first row transition metal oxides - $TiO_2, α-Cr_2O_3, β-MnO_2, α-Fe_2O_3, Co_3O_4, NiO, CuO, and ZnO$ - are calculated to demonstrate the accuracy of this approach. The theory is used to decompose the core-valence excitons into the separate components of the X-ray transition Hamiltonian for each of the transition metal oxides investigated. The decomposition provides a physical intuition about the origins of XUV spectral features as well as how the spectra will change following photoexcitation. The method is easily generalized to other K, L, M, and N edges to provide a general approach for analyzing transient X-ray absorption or reflection data.
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