Photoelectron Spectra of Gd 2 O 2 – and Nonmonotonic Photon-Energy-Dependent Variations in Populations of Close-Lying Neutral States
Photoelectron Spectra of Gd 2 O 2 – and Nonmonotonic Photon-Energy-Dependent Variations in Populations of Close-Lying Neutral States
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Gd 2 O 2 的光电子能谱和邻近中性态族群中的非单调光子能量相关变化
DOI：
10.1021/acs.jpca.0c11002
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发表时间：
2021
期刊：
影响因子：
--
通讯作者：
Jarrold, Caroline Chick
中科院分区：
文献类型：
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作者：
Mason, Jarrett L.;Harb, Hassan;Taka, Ali Abou;McMahon, Abbey J.;Huizenga, Caleb D.;Corzo, Hector;Hratchian, Hrant P.;Jarrold, Caroline Chick
光子能量在2.033 ~ 3.495 eV范围内获得的gd2o2光电子能谱显示出许多与光子能量相关的接近中性态。这些态的跃迁落在0.9和1.6 eV的电子结合能窗口内，归因于一个或两个电子跃迁到基态和低洼的激发中性态。另外，在2.1-2.8 eV的电子结合能窗口中观察到一个类似的电子态流形，它不能被分配给任何简单的单电子跃迁。这项研究扩展了先前对sm20 -三原子的研究，sm20 -三原子具有更复杂的电子结构，因为每个Sm中心都占据4f6亚壳层。由于Gd2O2和Gd2O2 -中半填充的4f7亚壳占据的电子结构更简单，因此在光谱中观察到的许多近距离跃迁可以更好地分辨，从而可以更详细地观察单个跃迁的相对强度随光子能量的变化。通过对许多可能的近距离电子态的支持计算，我们提出了可能导致观测光谱中光子能量依赖变化的强烈光电子-价电子相互作用的潜在描述。
Photoelectron spectra of Gd2O2–obtained with photon energies ranging from 2.033 to 3.495 eV exhibit numerous close-lying neutral states with photon-energy-dependent relative intensities. Transitions to these states, which fall within the electron binding energy window of 0.9 and 1.6 eV, are attributed to one- or two-electron transitions to the ground and low-lying excited neutral states. An additional, similar manifold of electronic states is observed in an electron binding energy window of 2.1–2.8 eV, which cannot be assigned to any simple one-electron transitions. This study expands on previous work on the Sm2O–triatomic, which has a more complex electronic structure because of the 4f6subshell occupancy of each Sm center. Because of the simpler electronic structure from the half-filled 4f7subshell occupancy in Gd2O2and Gd2O2–, the numerous close-lying transitions observed in the spectra are better resolved, allowing a more detailed view of the changes in relative intensities of individual transitions with photon energy. With supporting calculations on numerous possible close-lying electronic states, we suggest a potential description of the strong photoelectron–valence electron interactions that may result in the photon-energy-dependent changes in the observed spectra.