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首页> 外文期刊>The Journal of Chemical Physics >Valence photoelectron spectroscopy of N_2 and CO: Recoil-induced rotational excitation, relative intensities, and atomic orbital composition of molecular orbitals
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Valence photoelectron spectroscopy of N_2 and CO: Recoil-induced rotational excitation, relative intensities, and atomic orbital composition of molecular orbitals

机译：N_2和CO的价电子光谱：反冲诱导的旋转激发，相对强度和分子轨道的原子轨道组成

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摘要

Recoil-induced rotational excitation accompanying photoionization has been measured for the X, A, and B states of N~+_2 and CO+ over a range of photon energies from 60 to 900 eV. The mean recoil excitation increases linearly with the kinetic energy of the photoelectron, with slopes ranging from 0.73× 10~(-5) to 1.40× 10~(-5). These slopes are generally (but not completely) in accord with a simple model that treats the electrons as if they were emitted from isolated atoms. This treatment takes into account the atom from which the electron is emitted, the molecular-frame angular distribution of the electron, and the dependence of the photoelectron cross section on photon energy, on atomic identity, and on the type of atomic orbital from which the electron is ejected. These measurements thus provide a tool for investigating the atomic orbital composition of the molecular orbitals. Additional insight into this composition is obtained from the relative intensities of the various photolines in the spectrum and their variation with photon energy. Although there are some discrepancies between the predictions of the model and the observations, many of these can be understood qualitatively from a comparison of atomic and molecular wavefunctions. A quantum-mechanical treatment of recoil-induced excitation predicts an oscillatory variation with photon energy of the excitation. However, the predicted oscillations are small compared with the uncertainties in the data, and, as a result, the currently available results cannot provide confirmation of the quantum-mechanical theory.
机译：在60至900 eV的光子能量范围内，测量了N〜+ _2和CO +的X，A和B态伴随光电离的后坐力诱导的旋转激发。平均反冲激发随光电子的动能线性增加，斜率范围为0.73×10〜（-5）至1.40×10〜（-5）。这些斜率通常（但不完全）符合一个简单的模型，该模型将电子视为好像是从孤立的原子中发射出来的。这种处理考虑了发射电子的原子，电子的分子框架角分布以及光电子截面对光子能量，原子身份以及原子轨道类型的依赖关系。电子被弹出。因此，这些测量提供了用于研究分子轨道的原子轨道组成的工具。从光谱中各种光线的相对强度及其随光子能量的变化，可以进一步了解这种成分。尽管模型的预测和观测值之间存在一些差异，但是可以通过比较原子和分子波函数来定性地理解其中的许多差异。后坐力诱发的激发的量子力学处理预测了激发光子能量的振荡变化。然而，与数据中的不确定性相比，预测的振荡很小，因此，当前可获得的结果无法提供对量子力学理论的证实。

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