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Transuranium compounds probed by nonresonant inelastic x-ray scattering

机译：通过非共振非弹性X射线散射探测超铀化合物

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摘要

While x-ray absorption spectroscopy is mainly governed by electric-dipole transitions, the technique of nonresonant inelastic x-ray scattering (NIXS) offers the possibility to explore higher-order multipole transitions. These transitions obey different selection rules that can reach final states of higher angular momenta, opening complementary spectroscopic perspectives. Here, we investigate the suitability of NIXS to study transuranium compounds. We show that the K edge of the Be encapsulation can be practically fully excluded by using the imaging capabilities of the technique arising from the position of the signals on the multidetector. Experimental results for the multipole transitions at the actinide O_(4.5) edges (90-120 eV) in UO_2, NpO_2, PuO_2, and Pu_2O_3 are compared with multielectronic calculations. The spectral features are shown to be very sensitive to the ratio of the triakontadipole and octupole transitions, which could potentially be used to assess the radial expansion of the 5f wave function, which is expected to occur in covalent mixing with the O 2p states.
机译：虽然X射线吸收光谱法主要由电偶极跃迁控制，但非共振非弹性X射线散射（NIXS）技术为探索更高阶多极跃迁提供了可能性。这些过渡遵循不同的选择规则，这些规则可以达到较高角动量的最终状态，从而打开了互补的光谱学视野。在这里，我们调查了NIXS研究跨铀化合物的适用性。我们表明，通过使用信号在多探测器上的位置所产生的技术的成像功能，可以几乎完全排除Be封装的K边缘。将UO_2，NpO_2，PuO_2和Pu_2O_3中the系元素O_（4.5）边缘（90-120 eV）处多极跃迁的实验结果与多电子计算进行了比较。光谱特征显示出对三偶极和八极跃迁的比率非常敏感，可以潜在地用于评估5f波函数的径向扩展，该径向扩展预计会在与O 2p状态共价混合时发生。

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  • 来源
    《Physical review》 |2020年第7期|075103.1-075103.8|共8页
  • 作者

    M. Sundermann; L. Simonelli; S. Huotari; R. Eloirdi; G. H. Lander; R. Caciuffo; G. van der Laan;

  • 作者单位

    Institute of Physics Ⅱ University of Cologne Zülpicher Straβe 77 D-50937 Cologne Germany Max Planck Institute for Chemical Physics of Solids Nöthnizer Straβe 40 01187 Dresden Germany;

    European Synchrotron Radiation Facility (ESRF) B.P. 220 38043 Grenoble Cédex France ALBA Synchrotron Light Source E-08290 Cerdanyola del Vallès Barcelona Spain;

    Department of Physics P.O. Box 64 FI-00014 University of Helsinki Finland;

    European Commission Joint Research Centre (JRC) Directorate for Nuclear Safety and Security Postfach 2340 D-76125 Karlsruhe Germany;

    Magnetic Spectroscopy Group Diamond Light Source Didcot OX11 0DE United Kingdom;

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